Siegfried played college basketball for Ohio State University, and his tenure there overlapped with future Hall-of-Famers Jerry Lucas and John Havlicek. Siegfried, a junior high scoring guard, and Joe Roberts, a senior forward, were the two holdover starters when three outstanding sophomores, Lucas, Havlicek and guard Mel Nowell arrived for the 1959–60 season. Siegfried adjusted his scoring to allow for Lucas and Nowell while joining Roberts and Havlicek as a key defender. Siegfried was also an excellent free throw shooter few risked fouling. The Ohio State Co-Captain of the 1960 team, Siegfried played a key role in the Buckeyes run to the 1960 NCAA title. All five starters from that team later played in the NBA, which then had just nine teams and eleven players per team. Future coach Bobby Knight was a reserve on that team as well. Said Knight of Siegfried, "I never saw a better guard in the Big Ten than Larry Siegfried. He was a great player. He was tough as hell. He was physical, he could jump . . . if I had my choice of any guard who played in the Big Ten when I coached and everything else, I'd have a hard time picking someone else."