Van Gaal leaves after two years of a three-year contract, having discussed severance terms on Monday.
The former Netherlands boss, 64, is believed to earn around £6.4m a year.
Mourinho's appointment is expected to be confirmed after the 53-year-old Portuguese meets senior United officials on Tuesday.
Manchester United confirmed Van Gaal's departure at 20:30 BST, praising his "great professionalism and dignity throughout", while adding "a decision on a successor as manager will be announced soon".
In a separate club statement released at the same time, Van Gaal said he was "very disappointed" not to see out his "intended three-year plan".
United have made an offer to Ryan Giggs, Van Gaal's assistant, for him to stay at Old Trafford, but it is not known what role he would have and whether he would accept.
He arrived at Manchester United's training ground at 08:45 BST on Monday and left shortly before 17:00.
Forty-five minutes after his arrival in the morning, League Managers Association lawyer Paul Gilroy QC also drove into Carrington.
Gilroy is the same employment barrister who acted for David Moyes when he was sacked as manager by United in 2014.
He arrived at about 09:30 and was initially refused entry before being allowed in about 15 minutes later, refusing to answer questions about the reason for his presence.
According to his profile page on the Nine St John Street Chambers website, Gilroy has advised and acted for a number of football clients, including Roy Hodgson, Martin O'Neill, Sir Alex Ferguson, Harry Redknapp, Roy Keane, Roberto Martinez, Sam Allardyce, Brendan Rodgers, Alan Pardew, Nigel Pearson and Steve McClaren.
Van Gaal took control of United after leading the Netherlands to the semi-finals of the 2014 World Cup in Brazil.
BBC Sports.
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