Real Madrid are again three points clear at the top of the Primera Division after a 3-0 win over Levante on Sunday.
Carlo Ancelotti's men watched on Saturday as Atletico won at Celta Vigo to return to level points with them, before responding with a three-goal win.
Cristiano Ronaldo got them going before the break, with Marcelo and an own goal from Nikos rounding things off after the break.
The win also means they are four points clear of defending champions Barcelona and surely have to be considered the favourite of the three sides chasing the title.
Valencia and Athletic Bilbao shared the points in a 1-1 draw.
Valencia went in front through Paco Alcacer's 23rd-minute goal, but Aritz Aduriz's penalty half-an-hour later ensured both sides got something.
Espanyol gave their European hopes a further boost with a dominant 3-1 home win over Elche in the Primera Division.
The hosts needed just two minutes to open the scoring, David Lopez heading them in front from a corner. Diego Colotto got the second goal midway through the first half and Pizzi added a third in the second period, although Juan Rafael Fuentes scored an own goal to give the visitors a late consolation.
The victory means Espanyol can harbour serious ambitions about qualifying for Europe, now that they are just seven points behind sixth-placed Real Sociedad, while Elche are just three points above the bottom three.
Sevilla ensured their preparation for next week's Europa League derby clash with Real Betis was almost perfect with a 3-1 away win over Almeria in the Primera Division.
Carlos Bacca, Daniel Carrico and Kevin Gameiro all scored for Sevilla with Aleix Vidal claiming a late consolation for the home side as the result kept the pressure on sixth-placed Real Sociedad, who are two points clear of Sevilla in the overall standings.
The scoreline also left struggling Almeria in the bottom three but only one point from safety in a congested bottom half of the table.
On Saturday, relegation-battling Real Valladolid caused one of the upsets of the Primera Division season after inflicting a 1-0 defeat on reigning champions Barcelona.
The clubs were separated by 40 points and 16 places coming into the match but it was third-bottom Valladolid who emerged victorious thanks to Fausto Rossi's first-half strike.
Second-placed Barcelona had several chances to get back into the match but could find no way past Valladolid keeper Diego Marino, and Gerardo Martino's men could now find themelves four points adrift of Real Madrid if the pacesetters beat Levante on Sunday.
Two quickfire second-half goals from David Villa lifted Atletico Madrid to the top of the league standings with a 2-0 victory at Celta Vigo on Saturday evening.
With Barcelona having suffered a surprise 1-0 defeat at Real Valladolid earlier in the day and Real Madrid not in action until Sunday, Diego Simeone's side headed into the game at Balaidos knowing a win would put them at the summit.
The first half was a lacklustre affair but a different Atletico emerged for the second period and two goals in two minutes just after the hour mark from former Barca striker Villa sent Los Rojiblancos top - above Real on head-to-head record.
Rock bottom Real Betis claimed their fourth Primera Division win of the season as they secured a 2-0 victory against Getafe.
Struggling Betis took the lead in the 16th minute through Leo Baptistao before Ruben Castro made sure of the points before half-time.
The result leaves the Seville-based side at the bottom of the overall standings but they cut the gap to safety to eight points. Getafe remained in 15th place with 27 points.
First-half goals from Fran Rico and Youssef El Arabi gave a dominant Granada a morale-boosting 2-0 win over Villarreal on Saturday evening.
Rico scored from the penalty spot midway through the first period and then provided El Arabi with a key pass so the Moroccan could double the lead 10 minutes later.