Neurodegenerative diseases or acute injuries of the nervous system always lead to neuron loss and neurite damage. Thus, the development of effective methods to repair these damaged neurons is necessary. The construction of biomimetic materials with specific physicochemical properties is a promising solution to induce neurite sprouting and guide the regenerating nerve. Herein, we present a simple method for constructing biomimetic graphene oxide (GO) composites by covalently bonding an acetylcholine-like unit (dimethylaminoethyl methacrylate, DMAEMA) or phosphorylcholine-like unit (2-methacryloyloxyethyl phosphorylcholine, MPC) onto GO surfaces to enhance neurite sprouting and outgrowth. The resulting GO composites were characterized by Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, Raman spectroscopy, UV-vis spectrometry, scanning electron microscopy, and contact angle analyses. Primary rat hippocampal neurons were used to investigate nerve cell adhesion, spreading, and proliferation on these biomimetic GO composites. GO-DMAEMA and GO-MPC composites provide the desired biomimetic properties for superior biocompatibility without affecting cell viability. At 2 to 7 days after cell seeding was performed, the number of neurites and average neurite length on GO-DMAEMA and GO-MPC composites were significantly enhanced compared with the control GO. In addition, analysis of growth-associate protein-43 (GAP-43) by Western blot showed that GAP-43 expression was greatly improved in biomimetic GO composite groups compared to GO groups, which might promote neurite sprouting and outgrowth. All the results demonstrate the potential of DMAEMA- and MPC-modified GO composites as biomimetic materials for neural interfacing and provide basic information for future biomedical applications of graphene oxide.