Police reports show Smith called 911 from his car around 6 a.m. Sunday to say he was suicidal and needed help.
"A call came in from Greensboro," Archdale Police Chief Darrell Gibbs told Eyewitness News. "There was a gentleman driving on Interstate 85 southbound threatening to commit suicide."
Gibbs wouldn't say whether Smith was armed.
"I can't say right now about any kind of weapon," Gibbs said.
Authorities identified Officer Jeremy Paul Flinchum, 29, as the shooter.
When Flinchum arrived at the scene, investigators say there was an altercation that resulted in Smith being shot and killed. No additional details have been released.
Officials refused to release the 911 call or say if Smith acted in a manner that showed he wanted police to kill him.
"That's an angle we're looking at," Gibbs said. "That hasn't been confirmed yet."
Gibbs said the incident is a tragedy for everyone involved.
"The officer's family, you feel sorry for them," he said, "Also feel sympathy for the young man's family. I can imagine what they're going through. It's very devastating. It really is."
He also warned against anyone speculating about what may have happened.
"I hope people don't jump to conclusions on things," Gibbs said. "Wait 'til you get all the facts. People want to make up their own mind of what happened but it's not always as it seems."
Smith was a junior biology major and president of the Delta Kappa Epsilon fraternity.
Late Monday afternoon, the fraternity released a statement that said in part, "we are heartsick at the loss of our brother Courtland Smith. We are grieving deeply over this tragedy. He was a good friend and leader at the DKE house. We are focusing on Courtland and how much we loved him as well as grieving with his family."
A Delta Kappa Episilon alumnus said Smith set his career path his freshman year. The pre-med student wanted to be a pediatric cardiologist.
UNC Chancellor Holden Thorp also issued a letter to the student body informing them of the incident.
"We are deeply saddened by the tragic death of our student Courtland Smith, a junior from Houston, Texas," Thorp said in the letter. "There is nothing worse than losing a young person. Our thoughts and prayers are with his family and friends as they grieve and cope with such a great loss."
Thorp said grief counselors will be available to anyone who needs to talk.
The university has not released any other details or statements regarding Smith's death.