The operation targeted 80 properties, including brothels and pubs.
It also involved a raid by counter-terror police on the house of the leader of the Hell's Angel chapter in the city of Hanover.
The suspected crimes being investigated include people- and arms trafficking, prosecutors said.
The investigation, which also covers alleged cases of bodily harm and corruption, is primarily aimed at the Hells Angels chapter in the northern city of Kiel, they said.
A court ordered the chapter to be closed earlier this year.
Police are also looking for a corpse thought to be that of an ethnic Turkish man who crossed the bikers, German newspapers report.
The raid on the Hanover home of the Hell's Angels' leader in the city, Frank Hanebuth, involved the elite GSG 9 tactical police unit.
Officers armed with machine-guns and wearing balaclavas broke down a heavy wooden front gate and abseiled from a helicopter to gain entry to the property, media reports say.
They are also reported to have shot a dog belonging to Mr Hanebuth.
Mr Hanebuth, who is thought to have been in the property at the time, is accused of having known of, or even ordering, the crimes being investigated in connection with the Kiel Hells Angels, prosecutors said.
His lawyer, Goetz Von Fromberg, denied the allegations, saying Mr Hanebuth did not know anyone involved in the alleged crimes.
The motorcycle club  - the world's largest in terms of membership - has often been linked to organised crime, and is considered an organised crime syndicate by the US Department of Justice.
Police have raided dozens of properties across northern Germany as part of a major investigation into the Hells Angels motorcycle club, reports say.