Former Barcelona president Sandro Rosell and his wife were arrested on Tuesday as part of a money laundering investigation, Spanish authorities said.
The detentions are part of a money laundering investigation related to buying television rights for past matches of Brazil's national team.
Three other people have been detained, but their identities were not immediately released by authorities.
Police raided offices, homes, and businesses in Barcelona and other locations in Spain as part of "Operation Rimet," in reference to former FIFA president Jules Rimet.
Authorities said the operation used information from the FBI following the U.S. case against high-level FIFA officials in 2015.
Rosell's lawyer, Pau Molins, told Spanish media his client was "worried" and "surprised" but had done nothing wrong.
"His private actions in Brazil were completely legal," Molins said, according to Marca.
Rosell, a former Nike executive in Brazil, had close connections to the former president of the Brazilian football confederation, Ricardo Teixeira, who was mentioned in the indictment by American officials. Teixeira was also being investigated by Spanish authorities, and raids were also expected in Brazil.
Teixeira resigned from the Brazilian confederation in 2012 citing medical reasons amid widespread allegations of corruption and irregularities in his administration.
In the 1990s, Rosell negotiated several deals with Teixeira involving Brazil's national team and Nike, which remains the sportswear company used by the Brazilian team.
Several years ago, Rosell was formally accused by Brazilian authorities of using one of his companies to illegally benefit from a friendly between Brazil and Portugal in 2008. Rosell was cleared of any wrongdoing at the time.
In another high-profile case, Rosell resigned from his role as Barcelona president at the start of 2014 after it was alleged he misappropriated funds from the €57 million signing of Neymar from Brazilian club Santos.
Club member Jordi Cases claimed that the amount paid was more than the fee reported at the time and the case is ongoing.
Along with Neymar, Josep Maria Bartomeu, Barcelona, Santos and the company run by Neymar's parents, Rosell is due to stand trial on fraud and corruption charges after Cases' claims led to a complaint from Brazilian investment company DIS.
He and his wife were detained at their home in Barcelona during one of the police raids. They stayed at the location while authorities executed search warrants. Another home owned by Rosell was also searched by police.
Police left with Rosell nearly 10 hours after the raids started.