We report on a facile strategy for the direct and uniform deposition of a graphene/Co 3 O 4 thin film onto stainless steel substrate (SS) through cathodic deposition. Graphene oxides (GOs) were treated with poly(ethyleneimine) (PEI) which acted as a stabilizer and binder between GOs and cationic metal precursor. For the formation of PEI‐modified GOs (PEI-GOs) and Co 2+ complexes, the PEI-GOs dispersion was mixed with aqueous phase of Co(NO 3 ) 2 , then, the solution was used as the plating bath for coelectrodeposition. Results showed that the PEI-GOs and cobalt oxides were uniformly distributed on the surface of SS evidenced by field emission scanning electron microscopy. The prepared graphene/Co 3 O 4 film was employed as an anode material for lithium ion batteries, and it exhibited not only an enhanced cycleability but also high electronic conductivity.