Gould served as president for the Ms. Foundation starting in 2004. During her time as president, she expanded grantmaking to further include community project that emphasized sustainable change. When Hurricane Katrina hit in 2005, she immediately reacted by establishing the Katrina Women's Response Fund which granted $3 million in funds to organizations in Louisiana and Mississippi which helped low income women and women of color rebuild their communities. She has also been a contributor to the Huffington Post. In 2011, Gould was a visiting fellow at the Foundation Center where she worked with Atlantic Philanthropies for two years providing research and activities on social justice philanthropy. After her time at the Foundation Center, she served as associate director of Caring Across Generations, a campaign to help those provide long-term home care, from April 2012 to January 2014.