Marco Asensio and Vinicius Jr. scored second-half goals to earn Real Madrid a solid 2-0 win over struggling Valencia.
Gundogan was Pep Guardiola's first recruit when he took over the reins at City in 2016 despite the German being sidelined with a knee injury when he was signed from Borussia Dortmund.
Barcelona left it late to snatch a 1-0 win at Valencia on Sunday after Atletico Madrid's 2-0 victory at home to Deportivo La Coruna was overshadowed by the death of a visiting fan hours before kickoff.
Atletico Madrid stayed firmly on course for a surprise La Liga title triumph when Raul Garcia's header secured a 1-0 win for the leaders at home to seventh-placed Villarreal on Saturday.
City completed the treble of Champions League, Premier League and FA Cup titles, matching Manchester United's feat in 1999 and drawing comparisons with Guardiola's 2008-09 Barcelona team.
La Liga is set for one of its most thrilling finishes when Barcelona host leaders Atletico Madrid in a winner-takes-all showdown at the Nou Camp on the final day of the campaign on Saturday.
The win took second-placed Real to 62 points after 29 games, two behind champions Barca who beat Leganes 2-0 on Tuesday.
Barca looked set for a third consecutive league draw as they created scant opportunities but they were presented with the advantage of an extra man when Villarreal midfielder Daniel Raba was given a straight red card for a wild, studs-up challenge on Sergio Busquets on the hour mark.
The Italian coach considers that having healthy players, such as striker Karim Benzema, will be the key to face the schedule that awaits the Madrid side, who will be looking to defend their LaLiga, Spanish Super Cup and Champions League titles.
Karim Benzema scored twice after the interval with a penalty and a header from a corner to give Santiago Solari's side a 3-1 lead, after Raphael Varane struck in the 34th minute to cancel out Anuar Tuhami's goal for Valladolid five minutes earlier.
Barcelona's Lionel Messi was at the heart of another devastating attacking show.
Lionel Messi's late penalty saw bedraggled Barcelona scrape a 2-1 victory over Leganes on Sunday at a divided Nou Camp as the La Liga champions looked as if they had still not recovered from their harrowing midweek defeat to Paris St Germain.
Atletico Madrid put last week's painful defeat by Real Madrid behind them with a 3-0 win over Osasuna on Sunday that included two goals in the space of a minute and allowed them to return to the top four in La Liga.
Valencia continued their solid start to La Liga and climbed to second when recent Spain recruit Paco Alcacer set them on their way to a 3-0 win at Getafe on Monday.
Atletico Madrid maintained a two-point lead in La Liga with a 3-0 victory at Las Palmas and Barcelona and Real Madrid stayed hard on their heels with thumping wins over Athletic Bilbao and Sporting Gijon on Sunday.
Vinicius Jr scored a hat-trick in the first half as Real Madrid were crowned Spanish Super Cup champions
La Liga leaders Real Madrid were held to a frustrating 1-1 draw at lowly city rivals Rayo Vallecano on Sunday as Joselu's early strike was cancelled out by Raul de Tomas' penalty, a result that could spice up the title race with surprise package Girona.
Cristiano Ronaldo struck midway through the first half as leaders Real Madrid won 1-0 at Malaga in La Liga on Saturday, while Atletico Madrid stayed hot on their heels after Diego Costa netted in a 1-0 victory over Espanyol.
Sevilla missed a chance to get their La Liga campaign up and running when the Europa League holders surrendered the lead and were held to a 1-1 draw at Levante on Friday.
Real are third in the league standings with 54 points after 28 games, two behind second-placed Atletico Madrid who visit Athletic Bilbao later on Saturday and nine points behind leaders Barcelona who play at Real Betis on Sunday.
Cristiano Ronaldo ensured Atletico Madrid fans will have bitter memories of the last local derby at the Vicente Calderon stadium by scoring a hat-trick in a 3-0 win for La Liga leaders Real Madrid on Saturday. Ronaldo's deflected free kick put Real in charge in the 23rd minute in the first meeting of the teams since the Champions League final in May. The prolific Portuguese killed off Atletico's resistance by winning and converting a penalty in the 71st minute and capped a harrowing night for the home side by tapping in the third in the 77th.
Barcelona have been boosted by the successful return from injury of talismanic playmaker Andres Iniesta as they prepare to host city rivals Espanyol in La Liga on Sunday.
La Liga leaders Real Madrid returned to winning ways after two defeats, making light of playing most of the second half with 10 men to triumph 3-0 at home to mid-table Espanyol on Saturday.
Real Madrid made the most of Barcelona's slip-up to close to within one point of the La Liga leaders on Sunday with a 2-0 win over third-placed Valencia at the Bernabeu.
Promoted Alaves dealt champions Barcelona a shock 2-1 defeat at the Nou Camp on Saturday while Cristiano Ronaldo returned from injury to help Real Madrid thrash Osasuna 5-2 and go two points clear at the top of La Liga. With Lionel Messi, Luis Suarez and Andres Iniesta on the bench, Barcelona went behind to the visitors in the 39th minute before Frenchman Jeremy Mathieu equalised in the 46th. Ibai Gomez then scored the winner in the 64th.
Real Madrid forward Cristiano Ronaldo faces a race against time to be fit for the Champions League semi-final second leg with Manchester City on May 4.
Jose Mourinho believes winning La Liga was the toughest of the seven league titles he has sealed in coaching stints in his native Portugal, England, Italy and Spain, the Real Madrid manager said on Wednesday.
A late goal by Toni Kroos sealed victory as Real Madrid defeated an impressive Celta Vigo side 2-1 to win their first home La Liga game of the campaign on Saturday.
'Messi is a player that makes a difference in all games and in Clasicos he has always made a big impact but we will have to see if he is ready' 'You never know what can happen in these types of games and when you start as favourite it can often go wrong'
Thierry Henry was on target as Barcelona cruised to a 4-0 home win over Racing Santander on Saturday to move five points clear at the top of La Liga.
Title rivals Barcelona and Atletico Madrid stayed locked together at the top of La Liga after they played out an intense 0-0 draw with few genuine chances at the Calderon on Saturday.
Images from soccer matches held across Europe on Saturday, March 16.
Levante continued to defy their humble status as Valencia's second club when they beat Real Betis 3-1 to reclaim fourth place in La Liga on Monday.
Athletic Bilbao checked promoted Villarreal's impressive early-season run when they beat the team with the distinctive canary-yellow strip 2-0 at their new San Mames stadium in La Liga on Monday.
News of all that's transpired on and off the football field
A quickfire Arda Turan double, including an acrobatic bicycle kick, fired Atletico Madrid to a 3-1 home win over Espanyol in La Liga on Sunday and lifted the Europa League semi-finalists up to seventh.
Barcelona equalled a club record of 12 consecutive league wins as Neymar and Lionel Messi were among the scorers in a 6-0 thrashing of struggling Getafe 6-0 at the Nou Camp on Saturday.
Barcelona moved to within a whisker of a second straight La Liga crown when Lionel Messi, Bojan Krkic and Pedro earned a nervy 3-2 win at 10-man Sevilla on Saturday.
Barcelona coach Luis Enrique is expecting another gruelling game at Athletic Bilbao when the La Liga champions visit San Mames on Sunday.
Barcelona still have very little chance of catching leaders Real Madrid and securing a fourth successive La Liga title despite closing the gap to eight points, coach Pep Guardiola said on Monday.