The police force said in a statement that 250 officers are executing 52 arrest orders, 48 search warrants and 45 property-seizure orders in the states of Sao Paulo, Minas Gerais, Parana and Mato Grosso do Sul.
The operation is a continuation of a similar police action earlier this week that resulted in 28 arrests across seven Brazilian states.
The goal of the operation is to dismantle the financial nucleus of a branch of the criminal organization that manages its drug-trafficking business and orchestrates the laundering of criminal proceeds, the Federal Police said in a statement cited by Efe news.
Investigators, who launched their probe in November, say the suspects employed a money-laundering method that involved depositing small amounts of money in different accounts.
This enabled them to execute transactions without triggering the control mechanisms of financial oversight bodies, the Federal Police said.
The PCC branch carried out transactions involving over 7 million reais (some $1.78 million) during the course of the investigation.
The suspects arrested on Friday face charges of drug trafficking, membership in a criminal organization and money laundering, crimes that together are punishable by up to 33 years in prison.
The police and prosecutors have spent years on the trail of the PCC, a gang that was founded in the early 1990s at a Sao Paulo prison and continues to conduct much of its illicit activities from inside Brazil's penitentiaries.
It is involved in a range of crimes, from drugs and arms trafficking to cargo theft and fuel smuggling.
The PCC is one of several gangs vying for control of the drug trade in Brazil, a battle for supremacy that has touched off a war inside Brazil's prisons.
On July 29, a fight involving members of the Class A Command and Red Command gangs at a prison in the northern Amazonian state of Para left 58 inmates dead, 16 of whom were decapitated.
A day later, four inmates involved in that fight were killed by asphyxiation (apparently strangled by other prisoners) while being transferred to another penitentiary in that state.
( With inputs from IANS )