With his six-year contract having expired, Aurélio left Valencia to join English Premier League side Liverpool on a Bosman free transfer in July 2006, becoming the first Brazilian to sign for the club.

[1] He cited the chance to rejoin former manager Rafael Benítez as a key factor in his decision, telling the Liverpool Echo: "I am going to a new club in which the trainer knows me, to see if I can conquer the objectives I have set myself.

[11] Aurélio made his debut for the club in the FA Community Shield victory over Chelsea on 13 August[1] and played a key part in Liverpool's squad during his first season, notably providing two assists for Peter Crouch and Daniel Agger in a 4–1 win over fellow title contenders Arsenal on 31 March 2007.

[13] Aurélio scored again on 7 February 2009 against Portsmouth at Fratton Park with a free-kick into the bottom corner, getting his team back on level terms and helping Liverpool towards a 3–2 victory.

In the team's 1–1 draw with Chelsea in a Champions League semi-final first leg clash, Aurélio tore his adductor muscle after a forceful impact with Joe Cole and as a result was ruled out for the rest of the season.

[18] He made his first appearance in his second spell for the club in a pre-season game against Borussia Mönchengladbach the day after re-signing, coming on as a substitute and wearing the captain's armband for the closing stages of the match.

[19] New Liverpool manager Roy Hodgson declared his delight at being able to re-sign Aurélio and, during an interview with the club's television channel, said, "I was quite surprised when I found out he was fully fit and hadn't been offered a new contract, so I think it was a bit of an obvious thing to do.

On 24 May 2012, having only appeared twice in the Premier League the previous season, Aurélio returned to Brazil at the request of Vanderlei Luxemburgo to sign for Grêmio on a free transfer.

[8][22] However, his time at the club was marred by a torn cruciate ligament injury which saw him miss eight months of football, and he made only five appearances before announcing his retirement on 4 April 2014.

[23] In June 2003, Aurélio was called to represent Brazil senior team at the 2003 FIFA Confederations Cup by head coach Carlos Alberto Parreira but had to withdraw due to an injury.

[24] In October 2009, Aurélio would receive another chance to represent Brazil for friendly matches against England and Oman, but was not able to make his full debut as he had to withdraw from the squad again due to another injury.