The Argentine winger had a medical in Manchester on Tuesday and has signed a five-year deal.
Di Maria - described as "world-class" by United boss Louis van Gaal - is likely to make his debut on Saturday against Burnley in the Premier League.
The 26-year-old said United were "the only club that I would have left Real Madrid for".
The fee eclipses the £50m Chelsea paid Liverpool for striker Fernando Torres in 2011.
Di Maria added: "Louis van Gaal is a fantastic coach with a proven track record of success and I am impressed by the vision and determination everyone has to get this club back to the top - where it belongs. I now just cannot wait to get started."
Biggest transfer fees paid by a British club
£59.7m Angel Di Maria Real Madrid to Manchester Utd 2014
£50m Fernando Torres Liverpool to Chelsea 2011
£42.4m Mesut Ozil Real Madrid to Arsenal 2013
£38m Sergio Aguero Atletico Madrid to Manchester City 2011
£37.1m Juan Mata Chelsea to Manchester Utd 2014
£35m Andy Carroll Newcastle to Liverpool 2011
£35m Alexis Sanchez Barcelona to Arsenal 2014
United manager Van Gaal praised Di Maria as "a world-class midfielder" but added "most importantly he is a team player".
"There is no doubting his immense natural talent," continued the Dutchman.
"He is a tremendously fast and incisive left-footed player who puts fear into the most accomplished defence. His dribbling skills and his ability to take on and beat opponents are a joy to watch. He is an excellent addition to the team."
Di Maria is the sixth most expensive global signing ever, topped only by the big money paid out by Spanish giants Real and Barcelona.
Real signed Gareth Bale for £85m, Cristiano Ronaldo for £80m and James Rodriguez for £63m, while Barcelona paid between £65m and £75m for Luis Suarez, and £71m for Neymar.
United last broke the British transfer record when they paid Leeds £29.1m for former England defender Rio Ferdinand in 2002.
The Old Trafford club have spent £131.7m since last season, having bought left-back Luke Shaw, midfielder Ander Herrera and Di Maria's Argentina team-mate Marcos Rojo for a combined £72m this summer.
Di Maria was one of Real's most prominent players as they were crowned champions of Europe for the 10th time last season.
But his future in Madrid became increasingly uncertain as the club brought in James Rodriguez from Monaco and Toni Kroos from Bayern Munich.
Di Maria injured a thigh in Argentina's World Cup quarter-final win over Belgium, but was still named on the 10-man shortlist for the Fifa player of the tournament award.
He joined Real from Benfica for £36m in 2010, and won La Liga in 2012 and the Champions League last season.
Former Real president Ramon Calderon said on Sunday that he did "not like" the idea of Di Maria leaving, adding: "Normally a club who owns the very good players don't like to sell them."
However, in an open letter to Real fans published in Spanish newspaper Marca, Di Maria claimed that he did not want to leave the club.
"I want to make it clear that this was never my desire," he wrote, before claiming that "many lies" were spoken about his departure and admitting that he was saddened not to be offered a new contract.
"The only thing I asked for is something that would be fair," he added.
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