Officers found him in his 2.5 million euro Majorcan villa in Lloret.
In what was described as a major blow to the island's powerful German Mafia, some 100 members of the National Police and Civil Guard officers made 25 arrests in 31 raids in an operation directed by Spain's National High Court.
The raids led to the arrest of the most important Hells Angels figures in Europe, 49-year-old German Frank Armin Hanebuth.
Hanebuth considered by German police to be one of that country's most dangerous men according to Focus news magazine - was caught in a villa in Lloret when he was taken into custody.
One local police officer was also arrested in raids that capped off a three-year investigation.
Operation Casablanca targeted alleged drug trafficking, extortion, money laundering, and running of prostitution rings by the Majorca chapter of the notorious motorbike club.
Most of the club's members arrived on the island from Germany after authorities in that country cracked down on the group in 2009.
As part of their prostitution business on the island, the Majorca Hells Angels are said to have systematically performed cosmetic surgery on prostitutes.
This was done to make the product more attractive.
The Youssafi brothers apparently kept a tight rein on these operations, capturing women and only granting them a day off when they had earned a specific amount of money.
Several members of the Majorca chapter of the Hells Angels arrested on Tuesday were also wanted for kidnapping and homicide in Germany and it was also revealed by police sources yesterday they planned on laundering millions of euros by building a Formula One circuit on the island.
Furthermore, a hoard of weapons was seized during the raids, four motorbikes, nearly 50'000 euros in cash and various items of jewellry.
Nearly 100 bank accounts have also been frozen across Europe by the Spanish police working in cooperation with Europol and their Austrian, Dutch and German counterparts.
The gang has its origins in California after the Second World War and is thought to have between 2'000 to 2'500 members worldwide and the German Chapter apparently came to Majorca because they thought they would be able to keep a low profile and slip under the radar of the security services.