The North Carolina Highway Patrol says officer John Taylor was shot near milepost 172 at 2:24 p.m.
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.
Officers were looking for a man and a woman who were in the car. The man is described as a white and wearing a ball cap, Black Carhartt brand jacket with a hood, and blue jeans. He's about 6 foot and 200 lbs with an unshaven face and a buzz haircut. The woman is a white female with dark wavy hair, a dark shirt, black vest, and blue jeans.
Police Chief Jeff Hinton said at a news conference Thursday morning that the couple are considered armed and extremely dangerous. Anyone who sees them should call 911 right away.
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 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.
Hinton said there are no reports of other cars stolen in the Roanoke Rapids area, and law enforcement is assuming the suspects are still on foot and in the area.
Officers are using helicopters, tracking dogs, and are performing vehicle checkpoints. Hinton said police would also be going door-to-door to check on residents in the area.
"Everyone knows we have a job to do and we're doing it," said Hinton. "Everyone knows we're a small department, but we're stepping up to the challenge.