Police arrested the 26-year-old two weeks ago after, they say, two bystanders stopped an abduction in progress near the area of E. Rosemary Street and N. Columbia Street.
Detectives said Walker sprayed a 20-year-old UNC student in the face with pepper spray and then tried to drag her into his car.
Two brothers driving by saw what was happening and intervened.
Walker is charged with second degree kidnapping, assault on a female, and assault with a deadly weapon inflicting serious injury. Police found a loaded shotgun and a baseball bat in Walker's car. He allegedly had condoms in his back pocket.
Authorities later searched his home and seized several cameras - both digital and film, pornography DVDs, computers, notebooks, a safe, and two college IDs.
At a bail hearing, Judge Beverly Scarlett noted Walker may possibly suffer from mental illness. She called him a danger to women and set his bond at $5 million.
Since his arrest, Pitt County Chief Deputy James Tripp said Theodore Walker has been charged in connection with harming another woman in Pitt County.
In that case, Walker is charged with felony hit and run inflicting serious injury because he allegedly failed to stop and help the woman after she jumped from his car.
Orange County District Attorney Jim Woodall said evidence found in Walker's home linked him to the incident.
Two Chapel Hill teens have also come forward to report Walker tried to force them into his car the day before his arrest.