Capt Sir Tom, a World War Two veteran, became a household name in 2020 during the pandemic after raising millions for NHS charities by walking laps of his garden in lockdown.
After he died in February 2021, the charity watchdog opened an inquiry into the Captain Tom Foundation.
The commission's report found a "pattern of behaviour" in which the couple benefited personally from their association with the Captain Tom Foundation and said people "would understandably feel misled".
The commission called on the Ingram-Moores, who have already been disqualified from being charity trustees, to make a "suitable donation" to the charity in response.
A press release, various marketing materials and the prologue of Capt Sir Tom’s memoir stated that the books would be used to support the foundation.
A spokesperson for the foundation said they are “pleased with the Charity Commission’s unequivocal findings regarding the Ingram-Moores’ misconduct”.
Mr Gilbert added the foundation was a "lost opportunity".
"The point of the idea that we had was to create a charity that would address ageism, that would enable people to work when they were older, to create connections between older people who are isolated in the wider community," he said.
Responding to the charity watchdog's report, the Ingram-Moores argued it was a “breach of privacy” for the book deal to have been disclosed by the Charity Commission and said "significant fees" were paid to the literary agent, legal and PR professionals, with portions of the money used to support the Captain Tom Foundation.
The Ingram-Moores said there had been no misappropriation of funds from the charity and that they had been treated “unfairly and unjustly” by the inquiry.
Additional reporting by Jon Ironmonger