Moncrief was drafted in the third round, with the 90th overall pick, by the Indianapolis Colts on May 9, 2014. On May 30, the Colts officially signed him to his rookie contract. On October 26, 2014, in a game vs. the Pittsburgh Steelers, Moncrief scored his first NFL touchdown on a pass from quarterback Andrew Luck. In week 13, Moncrief had 3 receptions for a career-high 134 yards and 2 touchdowns to help the Colts beat the Washington Redskins 49–27. He finished his rookie season with 32 receptions for 444 yards and 3 touchdowns.