In this study, graphene aerogel (GA)-supported Fe₂O₃ particles with three-dimensional (3D) architecture was prepared by a one-pot hydrothermal process. Fe₂O₃ particles were dispersed uniformly on the graphene sheets, and the resulting composites self-assembled into a 3D network via hydrothermal treatment. This strategy provides a facile and environmentally friendly method for the large-scale synthesis of Fe ₂O₃/GAs without any additional reductant. As the anode material for lithium ion batteries, the Fe₂O₃/GAs in this study manifested an excellent reversible capacity of 995 mA h g^-1 after 50 cycles at a charge-discharge rate of 100 mA g^-1 and even delivered reversible capacity as high as 372 mA h g^-1 at a high rate of 5000 mA g^-1. The outstanding electrochemical performance of Fe₂O₃/GAs can be attributed to the synergistic interaction between uniformly dispersed Fe₂O₃ particles and graphene aerogel, in which a robust 3D framework of graphene provided highly conductive networks with a large surface area and short diffusion path length for the transport of lithium ions.