A police spokesman told Reuters in a phonecall that John Francis Morrissey, the high-profile ringleader of the gang and head of the Spanish operation, was arrested on Monday.
In total, three people were arrested in Spain and one in England, police said in a statement.
The ring was dismantled during a joint international Europol operation known as "Whitewall", they said.
The criminal network laundered more than 200 million euros in under a year and a half, or up to 350,000 euros a day, they said.
The money-laundering ring used the so-called "hawala" traditional money transfer system, widely used in Pakistan and the Middle East, that allows money to be exchanged between traders through a handshake, a piece of paper or on trust.
Police said that Morrissey had ties to the Irish "Kinahan Clan", a drug trafficking gang operating out of Spain's Costa del Sol, and was "dedicated to collecting large amounts of cash from criminal organizations that operate in our country".
He was arrested during an operation supported by operatives from the UK's National Crime Agency, the Irish Garda police, the American Drug Enforcement Administration, the Dutch police and Europol's Financial and Economic Crimes unit.
Police said they had started tracking the group after seizing cocaine and cash hidden in cars in Malaga last year.
The network traded in premium brands, one of them a luxury vodka brand promoted in top restaurants and nightclubs in southern Spain, but the Spanish tax agency said this trade "could in no way support" the ring's lifestyle, police said.
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