Venezuelan forces surrounded a house in the town of El Junquito, near the capital, Caracas, as they targeted the “cell” linked to pilot Oscar Pérez.
The authorities said they had arrested five people who they accuse of being part of a criminal group.
It is unclear what became of Mr Pérez.
Prominent government member Diosdado Cabello tweeted that Mr Pérez had opened fire on police.
Mr Pérez was wanted after he used a stolen helicopter to throw grenades at government buildings on 27 June.
In footage posted on social media on Monday, Mr Perez said he had offered to turn himself in but that he believed authorities were initially trying to kill him rather than negotiate his surrender.
“They’re shooting at us with RPGs [rocket-propelled grenades],” he said.
“There are civilians inside here. We said we’d turn ourselves in, but they don’t want to let us turn ourselves in. They want to kill us,” Mr Pérez added.
He then describes how those at the property with him were forced to “crouch down”, adding: “Now we’re negotiating.”
He ended the video, which he uploaded to the photo sharing site Instagram, with a message for the people of Venezuela, who he urged not to “lose hope”.
Pérez was on the run after launching a helicopter attack on the Venezuelan Supreme Court during opposition street protests last year.
He became the country’s most talked-about man and appeared in an online video on 5 July vowing to keep up his attacks on the government.
President Nicolás Maduro declared him a terrorist, accusing him of stealing a military helicopter and dropping grenades on the court to mount a coup.
Now in his mid-30s, Mr Pérez has been a member of the forensic police force, known as the CICPC, for 15 years.
The Venezuelan media emphasise that he is a highly trained agent, part of the Special Actions Brigade (BAE), where he is chief of operations for the Air Force division.
He has been pictured scuba-diving while brandishing a high-calibre weapon underwater and showing off his skills by shooting a target over his shoulder, behind his back, using only a make-up mirror as a guide.
The government has also accused Mr Pérez of having ties to the United States, specifically the CIA, which it also often says is trying to overthrow it.
As yet, Mr Pérez has no confirmed links with any international or domestic groups, although he has claimed to be part of an anti-government coalition of military, police and civilians. (Courtesy BBC)