Neville left his role as manager of England’s Women’s national team on Monday after almost three years in charge.
Inter Miami, who are co-owned by Neville’s former Manchester United teammate and England captain David Beckham, finished 10th in the Eastern Conference in their debut season in the MLS and dispensed with the services of Diego Alonso as manager at the end of the season.
"I am incredibly delighted for this opportunity to coach Inter Miami and to work with Chris and the entire ownership group," said Neville, who can start his new job once he receives a work visa.
"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."
Speaking of the arrival of Neville, along with the appointment of Chris Henderson as chief soccer officer (CSO) and sporting director, 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."