The multinational force said one of the Taliban leaders arrested in the raid in southern province of Kandahar's Panjwai district coordinated attacks on Afghan and coalition forces in the nearby Zharay district.
The other is believed to have served as a district Taliban chief for the past three months, NATO said. Two suspected insurgents were also detained.
NATO also said one of its service members was killed when a homemade bomb exploded in the country's south. It didn't say where exactly the early morning blast occurred. The service member's nationality was not released.
Seven service members with the international coalition have been killed so far this month, and 38 since the start of the year.
Last year was the deadliest of the nearly decade-long war for international troops, with more than 700 killed, compared to just more than 500 in 2009, which was previously the worst year of the war.
Another bomb in the eastern province of Nangarhar wounded two civilians when it exploded around 9:50 a.m., Afghanistan's interior ministry said. The ministry condemned the blast as "un-Islamic and inhuman" and said it was investigating.