Well-designed nanostructures have been regarded as keys for exploring new electrode materials for lithium-ion batteries. In this work, we reported a facile approach to prepare a novel flower-like clusters of Co3O4/C nanosheets via in situ pyrolysis of cheap inorganic-organic layered precursors. The as-prepared sample exhibits a two-dimensional architecture from well-graphitized carbon nanosheets embedded or anchored homogeneously by numerous Co3O4 nanoparticles (5–8nm). When used as an anode material, the composite displays a high reversible capacity (1082mAhg−1 at 100mAg−1), superior rate capability (531mAhg−1 at 2000mAg−1) and excellent cycling stability. More importantly, a very interesting and amazing microstructural evolution from the lamellar precursors to nanosheets has been unveiled for the first time, which not only manifests the rich in structural variation of inorganic-organic hybrids in pyrolysis process, but also opens up new perspectives on the rational design and controllable fabrication of novel functional materials by utilizing such lamellar hybrids.