The Chelsea boss's tongue-in-cheek gesture came during the Soccer Aid match which saw England lose 2-4 to the rest of the world (ROW) at Old Trafford.
Murs was proving a nuisance down England's left wing when the ROW manager stepped in to chop him down.
Wearing a loose tie, suit and trainers, Mourinho walked away grinning after bringing the Dear Darlin' singer down with the sneaky tackle from behind.
It was reminiscent of Boris Johnson's rugby tackle of a German player during the 2006 edition of Soccer Aid.
Murs, 30, had earlier tweeted a smiling picture posing with the Portuguese manager, adding: "Yep this happened last night!! Finally a picture with the special one".
The yearly match, which is held in aid of Unicef, features celebrities who wish they had grown up to be footballers and former football stars whose best days are behind them.
The over £4.2 million raised this year will go towards getting food, medicine and clean water to the world's poorest and most vulnerable children.
Managed by West Ham coach Sam Allardyce with the assistance of Take That star Robbie Williams, the England side combined the likes of Murs and comedian John Bishop with ex-players Jamie Redknapp and Matt Le Tisier
The rest of the world side featured Hollywood stars such as Jeremy Renner, Sam Worthington, James McAvoy and Kevin Bridges with Dutch footballing greats Edgar Davids, Clarence Seedorf, Jaap Stam and Edwin van der Saar.
Welsh mezzo soprano Catherine Jenkins added glamour to the occasion, singing Abide With Me before the game kicked off.
And celebs also graced the stands, with actress Kym Marsh tweeting: "At soccer aid with my gorgeous son!! He's so excited bless him".
Aside from the Mourinho/Murs fracas there was a more serious case of handbags at dawn when TV presenter Jonathan Wilkes clashed with Davids on a couple of occasions.
Wilkes drew first blood by tackling the Dutch midfielder from behind but Davids was quick to respond with a harsh tackle of his own and the two squared up.
Westlife star Nicky Byrne provided the most spectacular moment of the night after clinically lobbing England goalkeeper Jamie Theakston for the ROW to put themselves 2-0 up.
England pulled two back through former Liverpool player and Sky pundit Jamie Redknapp, with a swerving strike from outside the box, and recently retired former England international Kevin Phillips from the penalty spot.
But Dutch talent proved decisive and current AC Milan manager and four-time Champions League winner Seedorf scored twice to give the ROW their second Soccer Aid title.
Soccer Aid said a crowd of around 70,000 fans had turned out for the game.
The £4.2 million raised so far came from over £2 million in donations which will be matched pound for pound by the Government.
International Development Secretary Justine Greening added: "The incredible public response to Soccer Aid shows Britain at its best. We are backing the generosity of the British people by matching all donations to Soccer Aid pound for pound, helping Unicef double its impact."
"That means even more women giving birth safely and more children getting life-saving vaccinations and nutritious food in some of the world's poorest countries."