Tequinho and his two brothers, Edinaldo de Souza Brito Filho and Jacques Jeronimo Motta Neto, who were charged with murders attributed to the gang.
Police said Tequinho had connections with drug lords in the city of Rio and Sao Paulo.
The drug dealers ruled the traffic in three slums in Angra dos Reis, a tourist region known as 'the Green Coast' and famous for its beaches and islands.
Police chief Francisco Lopes said that the arrests did not conclude the investigations. The police still had court orders to arrest another 20 suspects, and would analyse what they had seized to identify other gangs operating in the region.
During the operation, about 70 officers from the state and federal police departments seized weapons, drugs, money and notes left by gang members.
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