Forty-three-year-old Renee Michele Phillips of Southampton, Pennsylvania was captured just before 11 a.m. Thursday in a wooded area along Three Bridges Road.
Roanoke Rapids police said Michael Eugene Edgerton, 38, also of Southampton, shot himself in the head.
Police said there was just a single shot and no officers fired their guns. A .380 caliber pistol was found with Edgerton.
Resident Donnell Thomas says he spotted Phillips walking through his backyard Thursday morning.
"I asked her, I said, 'Where are you going," he said. "She said, 'I'm just cutting through sir,' right then my instinct says this is the lady they're looking for."
Investigators say they believe the pair were behind the shooting of Officer John Taylor near milepost 172 at 2:24 p.m. Wednesday. He was taken to Halifax Memorial Hospital and later airlifted to Pitt Memorial where he was in critical condition.
The Highway Patrol says the vehicle the officer pulled over was reported stolen.
The green 1997 Geo Prism with a Pennsylvania license plate was later located empty in the parking lot of the Halifax Academy on Three Bridges Road near NC 903 in Roanoke Rapids.
Police Chief Jeff Hinton said at a news conference Thursday afternoon that the couple was eventually found not far away.
The manhunt for the suspects was relentless --troopers, dogs, helicopters-- from the moment Officer Taylor was shot.
Hinton said Officer Taylor was wearing a bulletproof vest. He was hit in the neck, upper chest, and hand. Despite that, Hinton said Taylor was expected to make a full recovery.
Hinton said passing motorists stopped to help Taylor and he was conscious enough - despite his injuries - to radio in for help and give a description of the suspects.
Hinton said Taylor had just walked up to the car from the passenger side when he was shot. Hinton said it happened in a matter of seconds.
Taylor is a veteran police officer who has served with Roanoke Rapids department for five years. He worked in law enforcement for four years before that. He is married with one child. Hinton described him as one of his more safety conscious officers who was ambushed in what began as a routine traffic stop.
Hinton said Taylor stopped the car for following another vehicle too closely and he didn't know it was stolen.
Phillips was being questioned by detectives Thursday afternoon. Hinton said charges were pending.
Hinton thanked all the law enforcement agencies that quickly pitched in to help his small department with the manhunt after Taylor was shot. He also thanked local businesses who provided food and other support.
The Police Benevolent Foundation has set up the "Officer John Taylor Fund" at BB&T Bank. Donations can be made at any BB&T Bank.
The Police Benevolent Foundation is also donations via text for Officer Taylor. You can help by texting the phrase COPS TAYLOR to 85944. A $10 donation will be made to the "Officer John Taylor Fund" through your cell phone bill.
A search of criminal records shows that Michael Edgerton has a criminal history in Pennsylvania. He has charges for theft, counterfeiting, and receiving stolen property. Renee Phillips also has theft charges dating back to earlier this summer. It's unclear what their relationship was.