The invention provides a graphite composite material. The graphite composite material comprises graphite and a lithium titanate layer coated on the surface of the graphite. The invention also provides a preparation method of the graphite composite material. The preparation method comprises the steps of mixing a coating layer raw material containing a dissolvable titanium source, a lithium source, graphite and a solvent in presence of a protective atmosphere; then heating the mixture; and then roasting the heated mixture to obtain the graphite composite material. As a thin lithium titanate layer with high Li+ conductivity and good degree of crystallization is coated on the surface of the graphite material, the cyclic performance of the graphite material is greatly improved, and the rate capability and the low-temperature performance are also facilitated.