She became involved in the national movement and joined activities sponsored by the fledgling SNCC such as Freedom Rides, community-action organizing, and voter registration drives and was arrested many times for participating in those activities. In the spring of 1961, Smith left her position as executive secretary of the Atlanta Student Movement to become the full-time southern campus coordinator for SNCC. This meant dropping out of college her junior year although she had intentions of returning. Once she joined the Freedom Riders, she immediately took part of a ride that was going from Nashville, Tennessee, to Montgomery, Alabama, on May 17, 1961. However, she was violently attacked and beaten in Montgomery and was arrested in Jackson, Mississippi, for traveling inflammatory. After the arrest, she used "jail no bail" by accepting 45 days in Parchman State Prison.