The arrested persons have been identified as Baiju Kumar and Bablu Kumar, Patna Senior Superintendent of Police (SSP) Jitendra Rana said.
One pistol and 13 cartridge shells have been recovered from the duo, both residents of Supanchak village under Fatuha police station in the district.
The two had been involved in several cases of attempt to murder and the Arms Act.
Another gang member, accompanying them, managed to escape on a motorcycle.
The gang, active around the state capital, had allegedly shot and injured three persons over the last five days.
The SSP said today's operation was conducted on a tip-off and the arrests will bring down crime on national highways around the state capital.