He made his first start of the 2020-21 season on October 17, 2020 due to injury.The match was a 1–0 win against Arsenal. On November 3, 2020, Cancelo scored his first Champions League goal for Manchester City in a 3–0 win against Greek team Olympiacos. His first league goal of the season happened on January 26, 2021. In that match, Cancelo scored the 2nd goal in a 5–0 win against West Bromwich Albion.