[10] On 30 January 2016, Angeliño made his debut for the first team in a 4–0 away win against Aston Villa, coming on in the 81st minute to replace Gaël Clichy in the FA Cup.

[11] He played for the club twice in the 2016–17 season, making his Champions League debut on 24 August, as a substitute in a 1–0 win over Steaua București.

[24] Angeliño made his debut in the 2019–20 Premier League season on 21 September, coming on as a half-time substitute for Benjamin Mendy in an 8–0 routing of Watford at the Etihad.

[25] On 31 January 2020, having made 12 appearances for Manchester City, Angeliño was loaned to German Bundesliga club RB Leipzig until the end of the season.

[30] In the final group stage match on 8 December, Angeliño scored his side's first goal in a 3–2 win over his parent club's bitter rivals Manchester United to knock them out of the competition.

[31] On 12 February 2021, Angeliño's loan to RB Leipzig was made permanent after he signed a four-year contract with the German club, for an undisclosed fee.

[35] A transfer fee of 6,000,000 euros was agreed to as a conditional purchase price should he sign on a permanent basis at the end of his loan.