Transition metal oxides have attracted considerable attention as possible electrode materials for lithium-ion batteries. However, poor electrical conductivity and volume change during cycling result in low rate capacity and rapid capacity fading, which hinder the practical applications of those electrodes. In this work, we report a facile approach to modify Co3O4 nanoparticles (NPs) by laser irradiation treatment. The structural and composition of the samples were studied by different techniques. The results show that the surface of the as-prepared particles transforms to a thin CoO layer, and oxygen vacancies are generated after the laser treatment. Compared to the as-prepared Co3O4 NPs, the laser treated sample shows a higher reversible capacity of 833.4 mAhg−1 after 100 cycles at a current density of 0.1 Ag-1. A capacity of 348.4 mAhg−1 can be obtained at a rate of 5 Ag-1. The unique microstructure that induced by laser irradiation in the Co3O4 NPs is responsible for the improved lithium storage properties.