In situ preparation of carbon nanotubes on the surface of spherical graphite particles is made by chemical vapor deposition, resulting in an “urchin-like” hybrid material. TEM and SEM images show that carbon nanotubes are herringbone with turbulent layered structure, less than 100nm in diameter and several micrometers in length in the average. The hybrid's use as an anode material in lithium ion batteries is examined using constant current charge–discharge tests, which prove that carbon nanotubes oriented on the surface effectively improve the reversible capacity. Cyclic voltammogram shows that there is no cathodic peak for the reaction of the Fe catalyst with Li+ in the charge-charge process in 0.0–1.6V vs. Li/Li+ potential range.