In order to improve the interface properties of composites, nanocarbons with different morphologies were deposited onto the surface of carbon fiber (CF) by controlling the process parameters using microwave plasma enhanced chemical vapor deposition (MPECVD) method. And then the multi-scale reinforcement was introduced into the interface layer of the CF/epoxy (EP) composites. Effects of different MPECVD technological parameters on the structural morphology of nanocarbon were researched by FESEM. The morphologies of nanocarbon on the interfacial shear strength (IFSS) were also studied by single fiber fragmentation test. And then, the relationship between interfacial properties and the micro-structure of interface region of nanocarbon-CF/EP was discussed. The results show that the morphologies of nanocarbon are changed significantly with the increase in deposition power. When the deposited power reaches 700 W, IFSS of nanocarbon-CF/EP composite increases by 118.85%, reaching 112.38 MPa.