Pedro Caixinha has resigned from Santos Laguna, a little over two months since guiding the team to the Clausura 2015 title.
The Portuguese coach's name has been linked to the vacant Mexico national team post since Miguel Herrera was released on July 28, but he had previously seemed to deny he was interested in the job.
Los Guerreros have started the current Apertura season poorly, with just one win from their first five games.
"After [carrying out] an analysis, I've decided to separate myself from the team," Caxinha said in a statement on Saturday. "The motives are secondary."
Santos had lost 2-0 to Club America on Friday evening in Estadio Corona, with Caixinha sent off from the bench by the referee in the first half.
Caixinha said the players asked him to stay and wished the club the best in the future, before leaving after just under two minutes in the press room at the club.
In almost three years at Santos, Caixinha won one Liga MX title, one Copa MX, the Campeon de Campeones trophy and guided the team to the playoffs in four of the five seasons he was in charge, reaching at least the semifinal in each one.