The appointment sees Neville reunite with his former Manchester United team-mate David Beckham, president and co-owner of the MLS club
Miami announced on Thursday that they had agreed to mutually part ways with Diego Alonso, the Uruguayan coach who oversaw their inaugural season.
The club finished 10th in the Eastern Conference on their MLS debut, making it to the playoffs play-in round, where they were beaten 3-0 by Nashville.
Now Neville, who leaves his role as head coach of England’s women’s national team with immediate effect, will take his first leading job in the men’s game.
However, he was set to leave the job this summer upon the expiry of his contract, with Sarina Wiegman, currently in charge of the Netherlands, to take over after the Olympic Games.
Beckham, the president and co-owner of Inter Miami, spent nine years playing in the Man Utd first team with Neville, the pair winning 12 major trophies together – including six Premier League titles and the Champions League.
They also played together for England, both making their senior international debuts in 1996.
Neville’s appointment creates a difficult situation for Team GB women’s football team, whom Neville was expected to take charge of at the Summer Olympics.
Speaking on Thursday, Sue Campbell, the FA’s director of women’s football, told BBC Sport: “We did make a decision that Phil would lead Team GB in November and we were moving towards an announcement when he started to have these discussions.
“Until those discussions are concluded, I can’t really say any more. If Phil remains, he will be Team GB coach. If he goes, we obviously have something to think about and work through. That is where we are.”
With Wiegman set to take a Netherlands team to the Games, her final task before becoming England manager, Team GB are now without a coach with just six months until the event takes place in Tokyo.
More to follow…