All-optically controlled devices are the attractive subjects due to their future applications in all-optically controlled networks and computers. In this work, two-dimensional (2D) graphite nanosheets are synthesized to improve organic photorefractive performance in the all-optical operation, i.e., the photorefractive performance under zero electric field. The synthetic process is performed by 2D-polymerizing electrophilic and nucleophilic carbon species under solvothermal effect, where [:C≡C:] 2− in calcium carbide is applied as nucleophilic carbon species and [C(Cl)] in carbon tetrachloride (CCl 4) as electrophilic carbon species. The polycarbonization reaction consists of 1D horizontal growth for nanoribbon and 2D vertical growth for single-layer graphene. Then, single-layer graphene nanosheets are aggregated via π-π stacking effect into 2D graphite nanosheets being composed of multilayer graphene nanosheets. Notably, the self-template characteristics induce the synchronous and alternate ongoing of three above processes. Interestingly, when these 2D graphite nanosheets are doped into organic photorefractive devices, the all-optically controlled photorefractive performance is effectively improved by enhancing the gain coefficient of two-beam coupling about 46.4% from 80.1 cm −1 of control device to 117.2 cm −1 of nanographite-doped device. This is attributed to the excellent electric conductance of 2D graphite nanosheets, which strengthens the charge separation under the nonuniform light field inside organic photorefractive devices. Then, the stronger built-in electric field will be induced so that the orientation enhancement effect is increased in organic photorefractive devices. This work provides an effective and facile approach to improve organic all-optically controlled photorefractive performance with 2D graphitic nanosheets. Weiwei Zuo and Mingming Li have contributed equally to this work.