The Greek footballer began playing for Liverpool on August 2020. He made his Liverpool debut in the EFL Cup, defeating Lincoln City 7-2 on September 24, 2020.

On the opening weekend of the season, 14 August 2021, he got his first league start in a 3-0 away win against Norwich City.  He followed this up with a man-of-the-match performance on August 21, assisting Diogo Jota’s goal in a 2-0 win over Burnley.

Tsimikas provided two assists in a 3-3 draw against Benfica in the quarter-finals of the 2021-22 UEFA Champions League on April 13, 2022, assisting Liverpool secure a spot in the semi-finals. He has amassed over 100 appearances on the field in his developing career.