The 22-year-old defender has signed a four-year contract, which keeps him at the Club until the summer of 2023.
"I am thrilled to have rejoined City, a side playing incredible football under Pep Guardiola," Angelino said.
"Watching them while playing in Holland has been a pleasure.
"City’s performances over the last two seasons have been incredible and I am very excited about returning and contributing to the Club’s bid for more success.
"I believe my own game can develop under Pep’s management and I am very confident that the Club will go from strength to strength over the next few years."
City Director of Football Txiki Begiristain added: “Angelino is a hugely talented young player and is an accomplished defender with great potential.
“Over the past year, he has gained excellent experience playing in the Eredivisie and the Champions League with PSV Eindhoven.
“We’re sure that he will bring additional defensive quality to our squad.”
Born in Coristanco, Spain, Angelino joined Deportivo La Coruna’s youth set-up at the age of 10, spending the next six years at the Club.
He made the move to City in January 2013, joining our Academy where he made a big impression at both Under 18 and Under 23 level as well as during a productive loan spell at our sister Club New York City in 2015.
After his return to City, Angelino made his first team debut in a 4-0 FA Cup win at Aston Villa in January 2016.
He then figured as a substitute in City’s 1-0 Champions League victory over Steaua Bucharest in August of that year before making his first start in a 2-1 League Cup success over Swansea City.
To help further aid his development and experience, Angelino then enjoyed separate loan spells with Girona and Real Mallorca in Spain before spending the 2017/18 campaign on loan in Holland with NAC Breda where he won four Rookie of the Month awards.
That was followed by his move to PSV Eindhoven in August of last year and a subsequent stellar campaign in the Eredivisie.
Angelino played 34 league appearances for PSV, scoring one goal and providing 10 assists.
He also impressed for PSV in the Champions League, playing in all six of their group games against Barcelona, Spurs and Inter Milan.
Everyone at City would like to welcome Angelino back to the Club and we wish him well during his time here.