The crash happened just before 6:30 a.m. on North Eastern Boulevard between Grove Street and Link Street.
Officers said 61-year-old Jonathan Hair stepped off the center median and was hit by a 2005 Nissan.
Hair was taken to Cape Fear Valley Medical Center in critical condition.
Southbound North Eastern Boulevard was closed between Grove Street and Person Street.
The road has since been reopened.
The department did not say if any charges would be filed.
Those with information should call the Fayetteville Police Department's Traffic Unit at (910) 433-1807 or Crimestoppers at (910) 483-TIPS (8477).