On September 18, 1960, in Buffalo's home opener, a 27-21 loss to the Denver Broncos, Carlton made history in the second quarter when he scored the team's first touchdown on a one-yard run. Carlton gained 1,010 yards from scrimmage (533 rushing- 477 receiving) and 11 TDs in the Bills first season.
Later he helped the Bills win back-to-back league championships in 1964 and 1965. Perennially among the AFL's top rushers, he led the league in rushing touchdowns in 1965 and was voted to the American Football League Eastern Division All-Star team in 1965 and 1966. Carlton was the Bills' all-time leading rusher during their AFL years, with a 4.1 yards per carry average.
In January 2012 it was announced that Carlton will be inducted into the North Carolina Sports Hall of Fame.