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She was a socialite who invented the modern-day bra. He was a playboy with a lust for literature. Together, they published some of the most beautiful books ever made, while living an outrageous life of bohemia.

After Nazi troops set up base in the French mill building Caresse and Harry Crosby had first leased as a holiday home in the '20s, Caresse was most distressed to learn that they'd painted over the white wall that had once doubled as her guest book. Among those who had autographed its walls were author D.H. Lawrence (he drew a phoenix) and Spanish painter Salvador Dalí (who intertwined his name with that of a Pulitzer Prize-winning American writer). While the soldiers' cover-up was hardly the Nazis' greatest act of art vandalism, it was an especially ironic one. Among the constellation of signatures they painted over was that of Eva Braun, later Hitler's wife, who had left hers alongside that of the Austrian big game hunter she was dating at the time.

"I wish I might have taken it with me when I left," Caresse wrote decades later, hinting she might have done something extraordinary when she left the mill in 1936 if she'd known what would happen four years later. Ridiculous as it sounds, taking an entire wall across countries was exactly the kind of gesture for which the Crosbys were notorious.

Harry and Caresse were a very attractive and preposterously well-connected couple, who scandalised upper-crust Boston with an adulterous affair, before settling in Paris. There, they lived a theatrically mad, bad and bohemian existence with a list of associates and collaborators that reads like a cultural index of the era.

They travelled widely and tried pretty much everything. Caresse and Harry were seen to embody the moneyed, decadent glamour of the roaring '20s and beyond. Today, bar a couple of ageing biographies and a few footnotes, they're all but forgotten; their once-famous names covered over by layers of history.

The Crosbys were so "modern" that their exploits are enough to make today's brightest young things feel old-fashioned. Opiates, exotic African holidays, flirtations with various faiths, riotous parties, seven-in-a-bed shockers, ominous tattoos, airplane joy-rides, gambling sprees ... they did it all.

Although their true vocation was being Caresse and Harry, the couple also ran the Black Sun Press, a small publishing house that printed exquisite editions by leading modernist writers, and commissioned some of the outstanding artists and illustrators of their day. Made with the finest paper and binding their money could buy – and laid out by an obsessively precise old typesetter – Black Sun Press books were often issued in minuscule numbers, with even smaller runs of special deluxe editions.

"If you're interested in the best of what came out of Paris at that time," says antiquarian books expert (and British actor) Neil Pearson, "a Black Sun book is the literary equivalent of a Braque or a Picasso painting – except it's a few thousand pounds, not £20 million."

The most beautiful of all their books, according to Pearson, is the Hindu Love Manual that Harry and Caresse found in Damascus and reprinted in 1928, in a release of just 20. It was bound in navy leather, which was stamped with gold in a nod to ancient Persian manuscripts. Its grey pages were handmade and decorated with a gold border, and each illustration in each copy was hand-coloured.

Unlike many of the pulp fictioneers and pornographers who published in Paris for purely business reasons, the Crosbys could afford to indulge their private passions. Indeed, two of the first three books they published were Caresse's first poetry collection, Crosses Of Gold, and Harry's Sonnets For Caresse. "They were publishing books of love poems to each other," says Pearson. "Of course, they wanted them to be beautiful."

The intensity of their lifelong affair started early. Harry told Caresse he loved her in the Tunnel of Love ride at Nantasket, Boston, on July 4, 1920. He had met her a few hours earlier at an Independence Day party. Harry's mother had invited Caresse, who was then called Polly Peabody. He was 22; she was 28. She was a sophisticated society star, inventor and one-time actress, and Harry was relentless in his pursuit of her.

After that first meeting, they couldn't keep away from each other. Two weeks later, they slept together – a terrible sin for two blue-blooded offspring of Old Boston who weren't married to each other, but one made far worse by the fact that Caresse was wed to someone else, and the mother of two young children.

Caresse Crosby was born Mary Phelps Jacob on April 20, 1891, a descendant of the first governor of the Plymouth Colony in Massachusetts, America's second permanent British settlement. In 1807, her great-great-great-great grandfather, Robert Fulton, created the first economically viable steamboat. The young debutante had her coming-out party in the winter of 1913 wearing a constricting corset-like contraption. Soon after, while dressing for another dance, Caresse looked at her dress and decided the effect of it was marred by the "boxlike armour of whalebone and pink cordage" protruding above its neckline. Inspired, she summoned her maid and told her she refused to wear it again. "Bring me two of my pocket handkerchiefs," Caresse recalled saying, "and some pink ribbon ... and bring the needle and thread and some pins." Caresse was mobbed after the dance by girlfriends who wanted to know how she'd moved so freely. A year later, she secured a patent for a purpose-built version of her "backless brassiere".

After setting up what she mischievously described as a "sweatshop" to manufacture her bras, she soon got bored and sold the design for $1500 to the Warner Brothers Corset Company, which is said to have made $15 million from it during the next three decades.

At the same time, she was seeing an old flame, Richard Peabody, whom she went on to marry the following January and have her first child with in 1916. Richard came back from WWI a hero, but ended up a broken alcoholic. His wife not only had to endure living with his parents, but also a husband whose primary nocturnal passion was the alarm bell he'd installed above their bed. As arranged with the local fire chief, this would ring whenever the emergency bell rang in the station, so Peabody could wake, dress in a firefighter's uniform and wear it while he watched real firemen tackle the flames.

Although he was also a war veteran and heavy drinker with eccentric habits, Harry was different to Richard. He never lacked passion, and he could start fires with just a hard stare – at least, that's what the many women who loved him said.

Caresse and Harry were a handsome couple. But Harry was the beautiful one. Although slight and pale, he had a distinctive blond hairstyle, a consuming gaze and enormous charisma, somehow exuding a presence that belied his stature. Later, he would accessorise this with black suits, black-painted fingernails and a black flower in his buttonhole. "He seemed to be more expression and mood, than man," wrote Caresse, "yet he was the most vivid personality I've ever known, electric with rebellion."

His rebelliousness wasn't inherited: Harry's pious, caring mother, Henrietta, loved nature and founded the Garden Club of America, and his banker father, Stephen, was a former college football star who lived for his Ivy League and Boston society connections. As a boy, Harry boarded at Boston's foremost prep school, St Mark's, and spent summers with his family in a house built by his uncle, Jack, aka J.P. Morgan, the most celebrated banker in American history. The teenage Harry was being groomed for Harvard, but he felt a conflicting pull when the US entered WWI.

In July 1917, Harry and several schoolmates set sail for France, where they were to serve in the relative safety of the American Field Service Ambulance Corps. He was soon in the thick of the bloody and exhausting business of ferrying those wounded in battle on the Western Front.

After the war, Harry returned to Boston and spent three years at Harvard. He left with a full-blown loathing for New England's obsession with etiquette, order and morals. He had seen too much in France to stay in what he called "dreary, drearier, dreariest Boston" and to put up with "Boston virgins who are brought up among sexless surroundings, who wear canvas drawers and flat-heeled shoes".

His taste for mischief and pretty girls was becoming an embryonic philosophy of living for the moment, whatever the risks and consequences. Any patience Harry once possessed was steamrolled by his lust for the now. Despite the social shame their affair brought on Caresse in Boston, Harry convinced her that they must live together. After her separation from Richard in February 1922, Caresse and her children left the US for Paris, where Harry took a bank job his family had arranged for him. They later married in September that year.

In 1924, the Crosbys released their first book. The following year, they each published their first collections of verse. Harry commissioned Alastair – a spectacularly camp German creator of beautifully decadent and Gothic fantasies – to illustrate his second collection, Red Skeletons. The book included Harry's most famously purple piece of adolescent expression, a sonnet to his corrupting hero Baudelaire. ("Within my soul you've set the blackest flag/And made my disillusioned heart your tomb/My mind which was once young and virginal/Is now a pregnant spleen-filled womb.")

Their new exotic location and Medici-like gestures made up for the variable quality of their poetry. Writers Ernest Hemingway and John Dos Passos were also in Paris, and had served with Harry during the war. Harry's cousin, Walter Berry, invited them to his salons, where novelist friends, like Henry James, Marcel Proust and Edith Wharton, would come to talk books in his unrivalled library.

The Black Sun Press published exclusive extracts from the most anticipated novels of the '20s and '30s, such as Finnegans Wake, as a beautiful book called Tales Told Of Shem And Shaun. The Crosbys' fastidious French printer even went behind their backs to ask its author, James Joyce, if he'd mind padding out the last page with a few lines to make it look prettier. He complied. Pablo Picasso, Caresse's first choice of illustrator, gladly met her, but ultimately turned down the offer on the grounds he didn't do portraits. Harry decided to pay another Black Sun Press writer, D.H. Lawrence, in gold coins, a gesture which he decided the author would appreciate. He did.

Max Ernst, the surrealist painter and a close friend of Caresse, provided haunting images for her tomes and the Crosbys branched out early into books about an art form then thought unworthy: photography. Harry developed a keen eye for photography during the second half of the '20s. According to Caresse, it was Harry's gift of a camera that inspired Henri Cartier-Bresson, who became the century's most noted photographer, to give up painting and return to photography.

Beyond the book business, the Crosbys' spectacular bacchanals, open marriage and prodigious ingenuity at marketing gave them a certain mystique. It was Harry who declared Caresse needed a new name and that he would choose it. Clytoris, an early suggestion, was sensibly saved for the family's second whippet (the first was named Narcisse Noir). They told Caresse's daughter, Polleen, that the dog was named after a Greek goddess.

But the good times were drawing to a close. In January 1929, Harry wrote to his father asking him "to sell $4000 worth of stock to make up for past extravagances in New York". In May, he sold another $4000 worth "to enjoy life when you can". In July, drunk on sherry cobblers, he sent his parents the following cable, "Please sell $10,000 worth of stock. We have decided to lead a mad and extravagant life."

Then, on December 10, 1929, six weeks after the first Great Crash saw the New York stock market lose $14 billion, Harry shot himself and one of his mistresses in a friend's studio apartment overlooking Central Park. He was 31 years old. A lover of dark mysteries to the end, Harry left no suicide note. The Herald Tribune reported "the authorities were unable to obtain information pertaining to a motive for the deaths". But there was plenty else to gossip about: Harry and Josephine Rotch-Bigelow – a young, wild, and recently married New Yorker – had smoked opium and drunk whisky. They were found fully clothed.

Harry's toenails were painted red and strange symbols were tattooed between his shoulder blades and on the soles of his feet. London's Daily Mirror speculated on psychological motives, while New York's Daily News blamed poetry and passion. Death itself had been the motive, others said, just as aspiring poet Harry's life had been his greatest artwork. He called cigarettes "coffin nails" and knew the drugs he took were dangerous. Harry had also asked the caretaker at the couple's holiday home (who was also a grave-digger) to erect a headstone – inscribed "Caresse & Harry" – in its grounds.

The Crosbys have probably been neglected in literary history because they were what Neil Pearson calls "dilettantes", frivolous interlopers in the serious world of 20th century literature. But, in their war on the repressive cruelty of social convention and deadening impact of puritanical morals, the Crosbys could be very cruel themselves. Harry didn't much care for children, and Caresse's son and daughter were shuffled around to keep them out of his way. During one Moroccan holiday, the couple took a 13-year-old girl called Zora to bed with them. Harry's one known homosexual experience – another holiday dalliance with a boy of unspecified age – left him in intense, if predictably short-lived, raptures. Their friends held "rape parties" and paid to see female circumcisions to add to their scandalous anecdotes.

When Caresse wrote her autobiography 25 years after Harry's suicide, she had moved on in many ways, starting pro-peace movements and artists colonies, getting to know (or collecting) T.E. Lawrence, F. Scott Fitzgerald, Allen Ginsberg and other artists and writers.

While living in Paris in the '30s, Caresse fell in with authors Henry Miller and Anaïs Nin, and taught them how to pen erotica. In 1937, at age 47, she had a short-lived marriage to a US football player, before settling in Rome in 1950. As for the enduring power of her and Harry's love, we'll never know. His diaries prove he gave her a unique status in relation to his mistresses, but Caresse still felt the need to doctor the less flattering entries about her (and some of Harry's tributes to other women) when they were published.

Yet Caresse, who died in 1970, aged 78, still bookended her life story with an extravagantly romantic gesture, the charming cruciform fusion of their names (right) that she and Harry devised early in their eight years together, and printed in their very first books.