Raisman is the latest gymnast to speak out against Nassar after Jessica Howard, the U.S. national rhythmic gymnastics champion from 1999 to 2001, and Jeanette Antolin, a Pan American Games silver medallist, also revealed they had been the victim of sexual abuse on the same programme in February.
Her "Fierce Five" teammate McKayla Maroney last month said Nassar had abused her.
Nassar has already pleaded guilty to federal child pornography charges and is in jail, awaiting a December 7 sentencing in that case.
Raisman, 23, is the latest member of the USA national team and the biggest USA gymnastics star to reveal being molested by Nassar, who is facing more than 20 counts of sexual assault.
Larry Nassar is accused of multiple sexual abuse on gymnasts for almost 20 years.
"I am angry. I'm really upset", the three-time Olympic champion told 60 Minutes. I can't ... every time I look at them, every time I see them smiling, I just think ... I care a lot when I see these young girls that come up to me, and they ask for pictures or autographs, whatever it is, I just ...
Aly Raisman won two silver medals at the 2016 Rio Olympics as well as team gold.
The 23-year-old, a two-time world team champion, revealed that she spoken to the Federal Bureau of Investigation regarding the claims of sexual abuse levelled at Nassar after she led the American team at Rio 2016. He was in a position of power, actually named the national medical coordinator for USA Gymnastics up until the summer of 2015.
Raisman - a 2-time national team captain who won 6 gold medals - opened up about the allegations to "60 Minutes". saying she met with the Federal Bureau of Investigation after the '16 Rio Olympics.
Raisman continued after Jon Lapook of "60 Minutes" noted her anger.
USA Gymnastics, in a statement to "60 Minutes", said it was "very sorry that any athlete has been harmed" and that "we want to work with Aly and all interested athletes to keep athletes safe".
Dantzscher also filed a lawsuit against Nassar in California last September as "Jane Doe".
Team USA Gymnastics released a lengthy statement about allegations in February, stating in part that "Regarding Dr. Larry Nassar, USA Gymnastics is appalled that anyone would exploit a young athlete or child in the manner alleged".
Raisman is the latest in a disturbingly long line of United States female gymnasts who have accused the disgraced doctor of inappropriate actions.