Nuno Espiritu Santo resigned as Valencia coach after his side's 1-0 defeat to Sevilla on Sunday night.
Nuno leaves the club after a season and 13 games in charge. He led the side to qualification to the Champions League during his first season at the helm at the Mestalla Stadium, only to see things fall apart in his second campaign, Xinhua news agency reported.
Sunday saw Jav Fuego and Joao Cancelo sent off in a chaotic display which leaves Valencia ninth in the BBVA Primera Liga table, while in Europe, successive defeats mean they have to win their last group game and hope that Zenit St Petersburg win in Gent in order to qualify for the last 16 of the Champions League.
This season had see Nuno under increased pressure from Valencia fans unhappy at the club's policy of signing players controlled by agent Jorge Mendes, who also represents Nuno.
"I am proud of having coached Valencia and grateful for the opportunity to have been their coach. I had spoken to club president (Lay Hoon Chan) and with owner, Peter Lim and also to them afterwards and we all agree the situation is not good and that we all have to do the best for the club. That has always been my intention," said Nuno in his last post game press conference.
Valencia's next match is a Copa del Rey tie against third tier side Barakaldo on Wednesday night.