The 49-year-old has won domestic league titles in his native Portugal, England, Italy and now Spain, becoming the first coach to achieve the feat, and led Porto and Inter Milan to Champions League triumphs in 2004 and 2010 respectively.
Real president Florentino Perez lured the self-styled 'Special One' to Spain from Inter Milan and has granted him unprecedented powers as the construction magnate and lifelong Real fan chases the elusive 'decima', or 10th continental crown.
In his second term at the helm of the world's richest club by revenue, Perez has splurged hundreds of millions of euros of Real's money on Cristiano Ronaldo, Kaka, Karim Benzema and others in a bid to end Barcelona's hegemony at home and abroad.
The job is only half done.
Real have fallen at the semi-final hurdle in their two Champions League campaigns under Mourinho, the first time to bitter rivals Barca and the second when they lost a penalty shootout to Bayern Munich at their Bernabeu stadium last week.
The only other silverware Mourinho has to show for his two seasons in the Spanish capital is the Copa del Rey, won last year when Ronaldo netted an extra-time winner against Barca, and some Madrid fans have yet to be convinced that he is the real deal.
Former England manager Fabio Capello won two La Liga titles in two stints at the Bernabeu and was sacked each time.
"It is nothing out of the ordinary for Madrid to win a Copa del Rey, a league and reach the semi-finals of the Champions League in consecutive years," a columnist in Real-cheerleading sports daily AS wrote on Monday.
"This is alright for a Madrid 'between the wars'. Of Mourinho I expected, and expect, more and I reckon those who whistled yesterday think the same," he added, referring to jeers heard around the Bernabeu when a small section of hard-core fans chanted the manager's name during Sunday's win against Sevilla.
Even if Mourinho has yet to deliver the European prize Perez and Real fans really hanker after, his achievement in leading the squad to the La Liga title at the expense of Barca should be given the credit it deserves.
He engineered the consistency required to get the better of one of the greatest teams in history with a campaign built around the awesome firepower of their front line.
Led by Ronaldo, Benzema and Gonzalo Higuain, Real have smashed the league scoring record of 107 set by John Toshacks's Madrid side in the 1989-90 season, hitting 115 goals in 36 matches with two still to play.
"That team spent five years playing together and this one has been together a shorter time so it deserves more merit," Emilio Butragueno, a striker in Toshack's team and now a Real director, told sports daily Marca recently.
"This Madrid side is devastating and they have a number of players within the team who can score goals."
Ronaldo and his great rival for the World Player of the Year title, Barca's Lionel Messi, have again conducted a personal duel to be the league's top scorer.
Messi's hat-trick against Malaga on Wednesday put him on a record 46 for the season, two ahead of Ronaldo.
The three forwards have greedily fed off the clever approach play of Mesut Ozil, Angel Di Maria and, less consistently, Kaka, and it is the first time that three players from one club have each scored 20 or more goals in a La Liga season.
For their part, Barca have continued to dominate opponents with their mesmerising possession game but have been more reliant than usual on Messi for goals as injury deprived them of Spain striker David Villa.
Madrid have lost only twice in the league, at Levante and at home to Barca, and drawn four times, but it is on the road where they have really bettered their arch rivals, dropping seven points to Barca's 16.
The Catalans were held to five draws, with an inability to finish off opponents proving costly as was evident in their Champions League semi-final demise against Chelsea.
With Real more consistent against the rest of La Liga some of the sting was taken out of the 'Clasicos'.
They met Barca six times in all competitions, losing three and drawing twice between the league, the Spanish Super Cup and the Copa del Rey, but Mourinho's side held the upper hand for the decisive league clash two weeks ago.
Real went into the match at the Nou Camp with a four-point advantage and still carrying some of the confidence from their thrilling Copa del Rey second-leg comeback to draw 2-2 in January, a major psychological boost despite their exit.
Ronaldo broke away to score the winner in a composed 2-1 victory for only a second triumph over Barca in 11 attempts during the Mourinho era.
Barca coach Guardiola's decision to step aside for next season, after winning 13 trophies in four years, prompted rejoicing in the Spanish capital with his assistant Tito Vilanova, whom Mourinho poked in the eye during a mass brawl at the start of this season, stepping up as an unknown quantity.
Mourinho knows the league title is expected as a matter of course next season and another failure to win the Champions League may prompt the mutterings from some quarters about his tactics and working methods to grow in volume.