Using the pressure-pulsed chemical vapor infiltration technique, thin pyrocarbon films were coated on the surface of the hard-carbon particles. The crystallinity of pyrocarbon shell was higher than that of the core carbon. The BET surface area and the pores with the diameter of 1.5–5nm were extremely decreased after coating with 7wt.% pyrocarbon. These changes in the nano-scaled structure of carbon surface could lead to the reduction of irreversible capacity. The cycleability was improved by pyrocarbon-coating, which would be attributed to the increase of the surface roughness on sub-micron scale by coating with the pebble-like pyrocarbon film to increase the adhesion among the particles by the organic binders.