Inter Miami confirmed the news on Monday, just hours after the Football Association announced the 43-year-old was stepping down from his role with the Lionesses with immediate effect.
The club are co-owned by Neville’s former Manchester United and England team-mate David Beckham.
Neville said in a statement published on Inter Miami’s website he was "incredibly delighted" to take up the new role.
He said: “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.”
Beckham said: “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."
The FA said it would confirm the name of an interim head coach to replace Neville soon..
The FA said last summer Neville’s successor would be Holland boss Sarina Wiegman, but the plan had been for her to take up her new position in September after managing the Dutch at the Tokyo Olympics.
It also remains to be seen what the FA do regarding a manager for the Great Britain team at the Olympics, a job Neville had been in line for.
Prior to the pandemic, the Lionesses were having a disappointing run with seven losses in 11 games.
Neville said in the FA’s statement announcing his departure: “It has been an honour to manage England and I have enjoyed three of the best years of my career with the FA and the Lionesses.
Baroness Sue Campbell, the FA’s director of women’s football, said Neville had made “a significant contribution during his three years with the FA."