Up to now, how to endow the electrode, composed of the high theoretical capacity materials, with high capacity and high capacity retention for lithium ion batteries (LIBs) is still a great challenge. Herein, for the anodes of LIBs, multi-layered GO-Fe3O4@PDA-PAM (graphene oxide-Fe3O4@polydopamine-polyacrylamide) composites, in which Fe3O4 nanoparticles (NPs) are confined by the polydopamine (PDA) shell and reduced graphene oxide (rGO) sheets, are fabricated through a green and scalable strategy. The multi-layered structure with confined Fe3O4 NPs endows the anodes with efficient cushion effect and good electrical conductivity, leading to a good lithium ion storage capacity. More interestingly, GO-Fe3O4@PDA-PAM flakes are generated driven by the electricity and grabbed by PAM linker to form the flower-like morphology and well-maintained during the following electrochemical process. The flower-like anode holds up the aggregation of active materials and provides abundant lithium ion diffusion pathway. Therefore, based on the entire composite mass, the flower-structured GO-Fe3O4@PDA-PAM anode displays a high reversible capacity, a good cycle reversibility (1204 mAh g−1 after the 100th cycle at 0.3A g−1) and an admirable rate performance (702 mAh g−1 at 1A g−1).