Having triumphed in South Africa four years ago and secured back-to-back UEFA European Championship titles, Vicente del Bosque's men were heavily fancied to win the tournament in Brazil.
However, Spain's campaign has proved to be disastrous as a 5-1 defeat to the Netherlands - who they beat in the 2010 final - in their opening game was followed by a 2-0 humbling by Chile on Wednesday.
It means Spain exit Group B with a whimper and with plenty to ponder as they look to return to the top of world football.
To do so, Chelsea boss Mourinho thinks that Spain must modify their famous tika-taka philosophy because other countries know how to play against the system.
"They scored one goal just with a penalty and they have zero points and they are already packing to go home," Mourinho told Yahoo Sport.
"I think it is fair to say that there is a big responsibility in Holland and Chile (for Spain's downfall). They did what I think in modern football you have to do - you have to be strategic.
"Holland and Chile were very good from a strategic point of view, and Spain couldn't cope with it in my opinion.
"People learn how to play against the best teams and when the best teams play always believing that their philosophy is the one, the other people learn.
"Spain was so amazing in the past four, six years - they were so amazing in the way that they were playing football - that people learn, people look, people study.
"(Netherlands coach) Louis van Gaal was brilliant in the way he analysed and he prepared the game against Spain but (Chile coach) Jorge Sampaoli even more.
"We have to be fair, and instead of saying Spain didn't play well - which I agree with - we have to be fair and say Chile did an amazing work and congratulations to the coach Sampaoli."
