A three-dimensional nanostructured graphene oxide–Mn3O4 hybrid was synthesized by a coprecipitation method and used as an anode material of lithium ion batteries, which reached an initial specific capacity of 1400 mA h/g. This method was developed to simplify the process of fabricating uniform composite nanomaterials for abundant applications. In this work, Mn3O4 particles were coordinately distributed on the surface of reduced graphene oxide nanosheets to avoid detrimental stacking of graphene layers by forming 3D nanostructures, as characterized by a scanning electron microscope. As demonstrated by the in situ observation of a scanning probe microscope, severe pulverization of Mn3O4 particles during charge/discharge processing was significantly abstained when graphene layers constrained swelling and shrinkage. The as-prepared graphene–Mn3O4 nanomaterials exhibited a large specific capacity of 949 mA h/g, high-rechargeable efficiency of ∼98%, and exceptional cyclic stability. After 100 constant-current charging/discharging cycles at 100 mA/g, the specific capacity remained at 792 mA h/g with a coulombic efficiency of 98.1%. Furthermore, the coprecipitation method proposed in this work provides a strategy to fabricate other nanostructured composites for different kinds of applications.