A law enforcement source familiar with the investigation told NBC News on Wednesday night that the pair was taken into custody south of Payson, Arizona, in an area known as Tonto Basin.
Blane, 56, and Susan, 59, escaped in Utah while being extradited back to Tucson from NY on August 26.
The Navajo County, Arizona, sheriff's office said in a statement that the Barksdales were arrested without incident and that the sheriff's office assisted the marshals service in the capture.
The reward for Blane Barksdale, called a "career criminal" by authorities, had increased to $25,000 with his addition to the 15 Most Wanted List, officials said earlier this week.
They were considered armed and unsafe after breaking free from two guards who were taking them from upstate NY to Tucson, Arizona to face murder charges over the killing of an elderly Vietnam veteran and burning of his house last April. They used a medical emergency to get the guards to pull over and then threw them in the back of the van, Gonzales said.More news: Democrats pressure Republicans by advancing gun control bill
More news: Meghan Markle set to attend Serena Williams' US Open final
More news: Apple Manipulates the App Store to Boost Its Own Products
The Barksdales drove the van with the three captives locked inside to Vernon, Arizona, where they got a red GMC truckthe U.S. Marshals Service has said. They then abandoned the van with the three locked inside and somehow evaded a sweeping manhunt conducted by multiple agencies, including the Federal Bureau of Investigation, the report said.
The Barksdales were located following what Gonzales on Monday said was a change in the direction of the investigation from a "rapid manpower search to an intense fugitive search". A third inmate who had been picked up in Kansas City was also in the van, but wanted "nothing to do with" the Barksdales' escape plan, Gonzales said.
The couple had been on the U.S. Marshal's 15 Most Wanted list when they were first captured. They then abandoned the van with their three prisoners inside.
The Barksdales were arrested in upstate NY in May following a nationwide manhunt, officials said.
But once the two unarmed guards opened the back door, the Barksdales attacked, he said. Evidence found there led detectives to conclude the blaze was set.