In this work, the construction of Co3O4 two dimensional (2D) nano-assemblies utilizing infinite coordination polymers (ICPs) as precursors was investigated, aiming at the morphology targeted fabrication and utilization of 2D materials. Based on the successful modulation of morphology, a rose-like Co based ICP precursor was obtained, which was further transformed into porous Co3O4 nanoflake assemblies with a well-preserved 2D morphology and a large surface area. The mechanism of the morphology modulation was illustrated by systematic investigation, which demonstrated the crucial role of a modulating agent in the formation of 2D nano-assemblies. In addition, the cobalt oxide 2D nano-assemblies are fabricated into a lithium anode combined with graphene, and the remarkable capacity and stability (900 mA h g(-1) after 50 cycles) of the resulting Co3O4/G nanocomposite indicates its potential in lithium battery applications.