The effect of atmospheric-pressure plasma treatment on high strength PAN-based carbon fibers had been studied in terms of fiber surface energetics and mode I and II interlaminar fracture toughness of unidirectional carbon fibers/epoxy matrix composites. The surface characterization of plasma treated carbon fibers was investigated by X-ray photoelectron spectroscopy (XPS) and contact angles. As a result, the plasma treatment changed the surface properties of the carbon fibers, mainly through formation of oxygen functional groups like hydroxyl, carbonyl, and carboxyl groups. According to contact angle measurements, it was observed that plasma treatment led to an increase in surface free energy of the fibers, mainly due to the increase of its specific component. Fracture toughness test results employing double-cantilever beam (DCB) and end notched flexure (ENF) specimens also showed that the increase in specific components or hydrogen bonding between the -OH groups on carbon fibers and the > O ring in epoxy matrix resins played an important role in improving the degree of adhesion at interfaces, resulting in an increase in the interfacial fracture toughness of the composites studied.