The rate performance of lithium iron phosphate (LiFePO4) is mainly limited by its poor electronic conductivity and slow Li-ion diffusion rate. Graphene-based materials are often compounded with LiFePO4 (LFP) to improve their rate performance, mainly because of their excellent electrical conductivity. Unlike most past composite work focusing on the conductive network between LFP and graphene, in this work, we further developed the functionality of graphene-based materials as nanoparticle carriers, where the nitrogen-doping strategy endows graphene with properties that make it an efficient structural regulation platform during the solvothermal process. Compared to reduced graphene oxide, not only does the nitrogen-doped sites confer more nucleation growth sites for LFP on the graphene surface during the solvothermal process, but also the localized formation of an EG-enriched microenvironment helps to further inhibit the in situ growth of LFP along [010]. The efficient structural regulation platform assisted the synthesis of (010)-oriented LFP with a smaller particle size, which further shortens the Li-ion diffusion paths. The optimized LFP composite electrode materials exhibit a discharge-specific capacity of 133.1 mA·h/g at 10C, which exceeds/is comparable to that of previously reported LFP compounded with graphene-based materials. This work broadens the functionality of graphene-based carriers and provides new ideas for the controllable synthesis of nanoparticles.