In his first season with Barcelona, Márquez appeared 21 times, helping the team to a second place finish in La Liga. During his second season, he was moved from his natural position as a center back to a defensive midfield role, due to injuries to players Thiago Motta, Edmílson and Gerard López. He completed a great season, being one of the main players that helped Barcelona win its 17th Spanish League on 14 May 2005 after a 1-1 tie with Levante. After an injury in his left knee, he returned after a month to play against Milan in the first leg of the 2006 UEFA Champions League Semifinal. Barcelona, playing away at the San Siro, won 1-0.
Márquez was present in the UEFA Champions League final on 17 May 2006 for Barcelona, in which they won the tournament over Arsenal. This achievement made him the first ever Mexican football player ever to ever win this competition, something Hugo Sánchez was not able to do during his time in La Liga with Real Madrid. After the 2006 FIFA World Cup, Barcelona extended his contract for the following 4 years to €38.5 million which will see his contract end in June 2010. Despite sustaining injuries, he was rumored to be up for sale at the end of the 2006-07 season. His future at Barça was up in the air until the 2007 Copa America, where Márquez regained his best form and was one of the best players of the competition, helping Mexico to an acceptable 3rd place.
In the 2007-08 season, Márquez got off to an excellent start, as he managed to form a solid partnership with new signing Gabriel Milito while captain Carles Puyol was out injured. However, constant injuries threw off his form. Márquez's success declined with the rest of the season leading Barcelona to end up in 3rd place after a miserable second half where injuries lead to his contribution being negligible. Even so, it appears new coach Josep Guardiola will continue to rely on his contributions; with the departure of Ronaldinho, Márquez has become the last original signing of the Rijkaard era to remain on the team. He appears to be Guardiola's first choice at center back along with captain Puyol for the 2008-09 season. On 13 December 2008, Márquez played his 200th match for Barcelona in the clash against Real Madrid, which they won 2-0. On 28 April 2009, Márquez got injured in a match against Chelsea in the semi-final of the Champions League. Márquez was told he needed surgery on his left knee, forcing him to miss the rest of the season. Barcelona would go on to win a historic treble after winning the 2008–09 UEFA Champions League, in which Márquez was present but was sidelined. Márquez also received an offer from Italian side Fiorentina. However, Márquez admits he would like to end his career at Barcelona and insists he is not concerned about the fact that his current contract runs out during the summer of 2010.
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