Mr Carter, 99, emerged from the wings of the Glenn Memorial Church at Emory University in a wheelchair to join the current president and first lady, as well as other former first ladies to pay his respects to his late wife of 77 years.
Rosalynn Carter died at 96 years old on 19 November, leaving behind a legacy of public service and humanitarian work to improve mental health advocacy, environmental conservation and more.
Mr Carter reflected on his late wife’s impact, saying she was “my equal partner in everything I ever accomplished.”
“She gave me wise guidance and encouragement when I needed it. As long as Rosalynn was in the world, I always knew somebody loved and supported me,” Mr Carter said of his wife’s passing.
The former president made the roughly 120-mile journey from his home in Plains, Georgia, to Atlanta to be present at Rosalynn’s memorial service.
Tuesday’s appearance marks only the second time Mr Carter has been seen in public this year. In September, Mr Carter and Rosalynn made a brief appearance at the annual Plains Peanut Festival.
None of the current or former presidents and first ladies spoke at the service, instead paying their respects and leaving.
The service reflected Rosalynn Carter’s down-to-earth preference toward celebrations. Her surviving grandchildren served as honourary pallbearers while her daughter, Amy Carter, and great-grandchildren presented readings.
Her son, James Earl “Chip” Carter, delivered a moving speech about his mother.
Rosalynn Carter’s longtime aide and friend Kathryn Cade as well as journalist Judy Woodruff also gave remarks.
The memorial service included music and arrangements from the Atlanta Symphony Orchestra, David Osborne, Garth Brooks and Trisha Yearwood. It included some of Rosalynn and Mr Carter’s favourite songs.
Before her passing, Rosalynn Carter was the second longest-living first lady.
Earlier this year, the Carter Center made public that Rosalynn had been diagnosed with dementia. She died only two days after they announced she entered hospice.
After the memorial service, Rosalynn Carter’s casket was taken back to Plains where her family and invited friends will attend a private funeral. Rosalynn will be buried at the Carter Home and Garden.