But with Hierro stepping down from his roles, the hunt for a permanent manager has started, with Roberto Martinez and Luis Enrique among the top contenders.
"After many kilometres of walking together, the Royal Spanish Football Federation and Fernando Hierro put an end to their relationship once the participation of Spain in the World Cup in Russia ended".
Spain, who won back-to-back European titles (2008, 2012) and the 2010 World Cup, are hoping to open a new successful chapter under Luis Enrique after three consecutive disappointing tournaments.
Hierro declined to return to his previous job as the federation's technical director and "will undertake new professional challenges", the federation wrote.
The challenge for the new boss is to take Spain back to the top of the worldwide game, as they have fallen in the group stages of the 2014 World Cup and at the last 16 stage at Euro 2016 and at this year's tournament.
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"The Federation wants to highlight the professional and human values of an extraordinary athlete".
Draws against Portugal and Iran in between a narrow victory over Iran were followed by elimination at the hands of Russian Federation in the last 16.
Luis Rubiales, the federation's president, sacked Julen Lopetegui on the eve of the World Cup after the Basque had agreed to join Real Madrid and he appointed Fernando Hierro for the ill-fated campaign in Russia.
The 50-year-old has made a decision to turn down his former role, despite being still under contract with the Spanish FA (RFEF).
Spain lead Group B in the opening round of the World Cup, beating Iran 1-0 and tying with both Portugal and Morocco.