In this work, oxyfluorination treatments on carbon fiber surfaces were carried out to improve the interfacial adhesion between carbon fibers and polarized-polypropylene (P-PP). The surface properties of oxyfluorinated carbon fibers were characterized using a single fiber contact angle, and X-ray photoelectron spectroscopy. The mechanical properties of the composites were calculated in terms of work of adhesion between fibers and matrices and also measured by a critical stress intensity factor (K(IC)). The K(IC) of oxyfluorinated carbon fibers-reinforced composites showed higher values than those of as-received carbon fibers-reinforced composites. The results showed that the adhesion strength between the carbon fibers and P-PP had significantly increased after the oxyfluorination treatments. As the theoretical and practical comparisons, OF-CF-60s showed the best mechanical interfacial performance due to the good surface free energy. This indicates that oxyfluorination produced highly polar functional groups on the fiber surface, resulting in strong adhesion between carbon fibers and P-PP in this composite system.