Angelino has joined RB Leipzig on a permanent deal from Manchester City after the Bundesliga club activated their £16.3m buy option in his loan deal.
The 24-year-old left back had been on loan at the Red Bull Arena since January 2020, but has now signed a four-and-a-half-year deal with Leipzig.
Angelino has often been used as a wing back by Julian Nagelsmann, with his new attacking freedom helping him to record eight goals and 11 assists this season.
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Despite becoming one of the German league's most productive full backs, Angelino failed to establish himself during two spells at City, making just 15 appearances in total.
He joined the club as a teenager from Deportivo La Coruna before embarking on loan spells at New York City, Girona, Real Mallorca and Dutch side NAC Breda.
Angelino then joined PSV on a permanent deal in 2018 but City used their buy-back option to re-sign him a year later.
However, he failed to convince Pep Guardiola and moved to Leipzig on loan after just six months back at the Etihad Stadium.
Bayern Munich are set to sign RB Leipzig defender Dayot Upamecano, according to their sporting director Hasan Salihamidzic.
Asked by German publication BILD if he could confirm an agreement had been reached between the clubs, he said: "I can, and we are very happy about that at FC Bayern".
The German champions appear to have beaten both Liverpool and Chelsea to Upamecano - one of the most sought-after defenders in the game.
Bayern chief executive Karl-Heinz Rummenigge previously told Sky Germany that both Premier League clubs were trying to sign him.
Salihamidzic added on Friday: "We had very good, intensive and professional discussions with Dayot and his agent Volker Struth over many months. We knew that we had very strong competition."