By the facile adhesion way, the novel composite complex by polydopamine (PDA) and magnetic graphite nanosheets (Fe3O4@GNSs) has been successfully synthesized. The resulting composite was characterized by means of scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectra, and Raman spectra, X-ray diffraction, X-ray photoelectron spectroscopy, and vibrating sample magnetometry. Meanwhile, the PDA functionalized Fe3O4@GNSs (Fe3O4@GNSs-PDA) was applied for Candida rugosa lipase (CRL) immobilization covalently without any toxic coupling agent. Combining the superior physical properties and chemical stability of Fe3O4@GNSs and the well biocompatibility, functional characteristics of PDA, the Fe3O4@GNSs-PDA composite displayed several advantages, including the high enzyme capacity, enzyme activity and stability and a decrease in enzyme loss. Our work demonstrated that the mussel-inspired Fe3O4@GNSs can be extended to many other applications such as biocatalytic, genetic and industrial.