Hybrids of Co(OH)₂ nanosheets (NSs) and Co₃O₄ nanoparticles (NPs) are synthesized by a facile hydrothermal strategy, wherein the Co(OH)₂ NSs form a flower-like structure and the Co₃O₄ NPs are embedded on the interlayer surfaces of the Co(OH)₂ NSs. The morphology, microstructure and composition of the hybrid can be tuned by the reaction time. When tested as anode materials for lithium-ion batteries, these ordered hybrid nanostructures of Co(OH)₂ NSs/Co₃O₄ NPs manifest significantly enhanced Li storage properties, including a high reversible capacity, long cycle life, and superior rate performance. The obtained promising performance could be attributed to the unique microstructure and the synergistic effect of the corresponding chemical composition in the nanocomposite.