The aircraft went down near Marine Corps Air Station Cherry Point in Havelock on Monday, according to a report by website military.com.
The pilot ejected before hitting the ground but had to be taken to hospital to receive treatment, the report added.
No civilian casualties or property damage were reported after the crash, according to a release by the Marine Corps, Presstv Reported.
"The crash site has been cordoned off by military officials," the USMC news release stated. "The cause of the mishap is currently under investigation."
Officials did not respond to questions about the time of the crash, the squadron the Harrier was assigned to or the nature of the flight and the possible reasons behind the crash.
Just days ago, an Air Force F-16 fighter jet crashed into a warehouse outside March Air Reserve Base in Riverside County in Southern California.
The pilot ejected before the crash but 11 people were injured inside the building. The aircraft was on a training mission at the time of the incident.
The Harrier crash brings to four the number of US military aircraft crashes this month. Two T-45 and T-6 training aircraft crashed earlier in May.
This latest mishaps are giving flashbacks to last year, when the US military lost numerous aircraft in crashes, including the loss of another USMC Harrier in Djibouti.