The English top flight, which has a dedicated team tackling piracy in order to protect the value of its broadcasting rights, referred the app called Mobdro to the Spanish authorities and Europol.
The league worked alongside the Alliance of Creativity and Entertainment (ACE) to investigate and refer Mobdro to the police.
As well as sports, Mobdro also illegally streamed a broad range of live television and video content across its channels.
Premier League director of legal services Kevin Plumb said: “Mobdro’s criminal enterprise amounted to long-running and large-scale theft.
“These raids show we and our colleagues at ACE are committed to taking action against piracy, regardless of location.
“The protection of our copyright is hugely important to the Premier League and our broadcast partners, as well as the future health of English football.”
The Premier League wrote to the US Trade Representative in February last year urging it to keep Saudi Arabia on a watch list because it said the country remained a centre for piracy.
The Middle East country was found by the World Trade Organisation in June last year to have facilitated the activities of the pirate network beoutQ, which illegally broadcast matches from the Premier League and other competitions.
The Qatar-based broadcaster beIN SPORTS renewed its rights deal with the Premier League for the Middle East and North Africa (MENA) region through to 2025 in December last year, which the company openly stated was a show of faith in the league’s efforts to combat piracy.
The chairman of the beIN Media Group, Nasser Al Khelaifi, said at the time: “This deal demonstrates that rights holders who do the most to protect their intellectual property also do the most to protect the value of their media rights.”