Vicente Del Bosque believes Catalunya has earnt the right to question its position as part of Spain and hopes to see an improvement in the situation as soon as possible.
The past month has seen mass demonstrations in the streets of the autonomous entity, with reportedly up to as many as 1.5 million people marching in support of the area's push for independence.
"The Catalan people have expressed freely, peacefully and without aggression. We must be tolerant and understand that," he told reporters.
"I talk about football. Maybe it's utopian, but if we could help relations [between Catalunya and the rest of Spain] get better and more cordial, I'd feel as happy as I was after winning the World Cup."
Del Bosque also spoke about ex-Barcelona coach Pep Guardiola, who recently conceded that he could be interested in managing the Spanish national team in the future.
"I think he has many qualities and is part of what Spanish football is about. He was a man committed to the Spanish national team," he remarked.