With continuous development of electrochemical energy storage technologies, electrode materials play increasingly important roles in promoting batteries capability. It is very desirable to construct novel materials in enhancing high-rate performance because serious energy attenuation with charge-discharge cycles under high current density has being become the bottleneck of secondary battery technology. We develop a Ni-Al LDH/graphene superlattice composite which is constructed via the electrostatic self-assembly of the delaminated positively charged Ni-Al LDH platelets and the exfoliated negatively charged graphene. The Ni-Al LDH/graphene superlattice composite exhibits excellent rate performance that retains both high capacity and steady cycle life at large charge-discharge current, and is supposed to serve as a promising high-rate battery cathode.