“She is the No. 1 most-wanted domestic terrorist, as she has been crucial in managing the Revolutionary Struggle, but more specifically in recruiting,” Mr. Chronopoulos said in a phone interview.

Starting in 2010, Ms. Roupa and Mr. Maziotis served 18 months in pretrial detention, the maximum possible, on terrorism charges. They were released in 2012 and were required to check in with the local police once a week, but instead they went on the run. In 2013, they were sentenced in absentia to 50 years in prison. Another leader of the group, Costas Gournas, also received a 50-year sentence.

The group, which had been thought to be inactive, claimed responsibility for an April 2014 bomb that was placed in a parked car in central Athens. No one was injured in the attack. That July, Mr. Maziotis was arrested after a shootout with the police in central Athens in which he and three other people — a police officer, a German tourist and an Australian tourist — were injured.

Early last year, the police said, Ms. Roupa tried to free Mr. Maziotis and other prisoners. She rented a helicopter and tried to force the pilot at gunpoint to fly over the prison where they were being held. But the pilot refused, and in the struggle that followed, he managed to regain control and land the helicopter. Ms. Roupa ran off.

“Over the last year, the police had been collecting significant information and indications leading us to the municipalities of southern Athens,” Mr. Chronopoulos said on Thursday. The police monitored the house over the past three days, he said, and on Wednesday evening, “when we were made sure that it was indeed Pola Roupa living in that house, we decided that it was time to go in with the raid.”