The news comes after an announcement from the Football Association earlier on Monday that Neville was stepping down as England Women head coach with immediate effect.
Inter Miami are co-owned by Neville's former Manchester United and England team-mate David Beckham, who is also his fellow co-owner of League Two side Salford.
Neville said in a statement on Inter Miami's official website: "I am incredibly delighted for this opportunity to coach Inter Miami and to work with Chris (Henderson, the club's new chief soccer officer and sporting director) and the entire ownership group.
"This is a very young club with a lot of promise and upside, and I am committed to challenging myself, my players and everyone around me to grow and build a competitive soccer culture we can all be proud of.
"This fantastic soccer-loving market deserves consistent performances and a winning mentality, and I look forward to getting to work."
The club had confirmed the appointment of former USA midfielder Henderson shortly before announcing Neville's.
Beckham said: "I am very happy with the leadership group we have established to lead the team as we turn the page following our inaugural season and look forward to having Chris and Phil join us soon.
"I have known Phil since we were both teenagers at the Manchester United academy. We share a footballing DNA having been trained by some of the best leaders in the game, and it's those values that I have always wanted running through our club.
"Phil has deep experience in football, as a player and as a coach at both club and international level, and over his career he has worked with many of the finest managers and players in the game.
"I know his qualities as a person, his decency, loyalty and honesty - and his incredible energy and work ethic. Anyone who has played or worked with Phil knows he is a natural leader, and I believe now is the right time for him to join."
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