Sources say his son Gorka and another federation official were also detained in the probe, which notably focuses on allegations of skimming profits from international matches.
Vice President of UEFA and president of the Spanish Football Federation (RFEF), Angel Maria Villar, was detained by police on Tuesday as part of a corruption probe, a judicial source said.
Villar, 67, was being held on suspicion of abusing his position to embezzle funds from the federation, among other charges, the source said.
Villar arrested today apparently due to use of RFEF money to secure support for his re-election from different regional presidents— Dermot Corrigan (@dermotmcorrigan) July 18, 2017
His son Gorka and another RFEF official were also detained in the probe, which notably focuses on allegations of skimming profits from international matches, a source said.
The RFEF could not be reached for comment.
TRT World's Lance Santos has more.
Villar, a one-time midfielder for Athletic Bilbao, has been the head of the federation for nearly 30 years.
He was fined $26,000 last year by FIFA's Ethics Committee for failing to co-operate with an investigation into the contest to host the 2018 and 2022 World Cups that triggered the worst crisis in the soccer world governing body's history.
The investigation into Villar is already several months old and stems from claims raised by the Spanish state's sports body in early 2016, police said.
Spain's political and financial crimes court said it is directing the probe into allegations of "collusion, fraud, embezzlement and presumed forgery."
At least four people were arrested in Tuesday's raids, according to police.
They included another member of the RFEF and an executive from the Tenerife football association, who are accused of misappropriating funds and syphoning them off to a company they both manage, police said.
Police who carried out raids on the federation headquarters and other locations related to the probe said that Villar is suspected of organising international football matches as part of a scheme to embezzle profits for the benefit of his son.
Inigo Mendez de Vigo, a spokesman for the Spanish government, told public television in response to the Villar arrest that "no-one is untouchable and everyone must obey the law."
The RFEF is due to hold an assembly on July 20 to approve the match scheduled for Spain's next La Liga football season, a meeting usually presided over by Villar.