Fernando Hierro, who led Spain at the 2018 World Cup, has stepped down as coach and will not return to his former role as sporting director.
Hierro was placed in temporary charge of the team after Julen Lopetegui was sacked on the eve of the tournament.
However, the 2010 world champions were knocked out on penalties by hosts Russia in the last 16.
According to the Spanish football federation, (RFEF), Hierro decided to seek new horizons.
A statement said the former Real Madrid player had “declined” to return to his previous role and has opted to “undertake new professional challenges”.
In Russia, Spain topped Group B under Hierro.