The chase started shortly after 3:30 p.m. - after officers began investigating a suspicious male in a parked vehicle in the 9400 block of Glenwood Avenue.
Authorities say Kasim Jerell Miller, 37, attempted to strike an officer with his vehicle, then fled and refused to stop.
According to eyewitnesses, dozens of patrol cars chased the suspect on I-540, then onto high-volume surface streets, including Creedmoor Road, Strickland Road and Falls of Neuse Road, before the pursuit ended on Ray Road, where he crashed into another car, ran off the road, and hit a tree.
Police say Miller then jumped from his car and ran from officers, before being captured a short time later.
There were three people in the car that was hit, including two children. None of them were hurt.
There was also a separate crash on Falls of Neuse Road, involving an RPD cruiser and another vehicle.
No one was seriously hurt in that impact, either. The officer was apparently responding to assist other units involved in the pursuit.
Investigators are trying to find the driver of an unknown vehicle who officers say likely witnessed events related to the second crash on Falls of Neuse Road.
The unknown vehicle is described by witnesses as a tan or gold small SUV, possibly a Honda Pilot or Chrysler PT Cruiser.
Authorities are asking that driver or any other witnesses who have yet not spoken to Raleigh Police to call (919) 996-1188.
State Highway Patrol troopers and Wake County Sheriff's deputies also assisted in the chase.
Police have charged Miller with assault with a deadly weapon, fleeing in a motor vehicle, hit and run, resisting a law enforcement officer, possession with intent to sell or deliver cocaine, possession with intent to sell of deliver marijuana, and possession of drug paraphernalia in connection with the investigation.
Miller has been transported to the Wake County Jail.