Graphene/α-MnO2 nanocomposites (GMC) with high performance as anode material were synthesized by a facile green procedure, in which we reduced graphene from graphene oxide and prepared the GMC simultaneously through a conventional hydrothermal route. The samples are systematically investigated by X-ray diffraction analysis, Raman spectroscopy, FT-IR spectroscopy, field-emission scanning electron microscopy, and transmission electron microscopy. The GMC presents a good reversible specific capacity of 998mAhg−1 at a current density of 60mAg−1 after 30 cycles and excellent rate capabilities of 590mAhg−1 at a current density of 12Ag−1. The present results indicate that GMC nanocomposites have enormous potential for application in lithium-ion batteries.