"Each of these people was a victim of either crime or an accident - and we need to show them some due respect," Ms Carroll said.
"Now it's time to close this chapter and hand them back, where we can, to their relatives and family. Quite simply, it's the right thing to do."
Twenty aborted foetuses and four babies that were infanticide victims were held at the museum too. Skeletal remains were also bought from suppliers.
Five confirmed murder victims and one adult who died accidentally were kept at the museum.
Ms Carroll said the museum also kept remains of seven adults who died in mysterious circumstances.
She said in the new YouTube video she used official records and newspaper articles to learn more about the victims. Ms Carroll then contacted the Department of Internal Affairs to trace more information about relatives of the deceased.
These next of kin were now talking to police about the best way to honour their relatives.
Some remains will be cremated or buried in local cemeteries.
Ms Carroll said it was an "extremely spiritual" experience to care for the remains.
She often felt outraged that offenders in some cases were remembered but the victims weren't, she said.
"I realised that they hadn't been revered in death the way they should have been. And these people had died tragically, so it was really important to give them back some dignity, to show them some care, and to look after them."