In this paper, a Cu, N co-doped TiO2 nanosheet with increased visible light photocatalytic activity was successfully synthesized using a biomimetic layer-by-layer deposition process. The polymer, branched-polyethyleneimine (b-PEI) was used as an induction agent for the hydrolysis of titanium bis(ammonium lactato)-dihydroxide (Ti-BALDH) as well as for a nitrogen resource, and the graphene oxide (GO) was used as a two-dimensional nano-template. The positively charged b-PEI will bind to the negatively charged GO and titania. In a typical layer-by-layer deposition process, GO nanosheets are exposed in an alternating fashion to aqueous b-PEI, CuCl2 and Ti-BALDH solutions, thus, making the layer-by-layer deposition of a conformal b-PEI/Cu-Ti-O coating on the GO. Subsequent b-PEI and GO pyrolysis at 550 °C under air yielded Cu, N co-doped TiO2 nanosheets. The materials obtained were comprehensively investigated by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, UV-Vis diffuse reflectance spectroscopy, Raman spectra, photoluminescence spectra and electron paramagnetic resonance. The Cu, N co-doped TiO2 nanosheets showed obviously enhanced photocatalytic activity which was evaluated by degradation of methylene blue under visible light irradiation. This research might provide some new insights for the "green synthesis" of the simultaneous doping of two kinds of foreign atoms into TiO2 with controlled morphology and photocatalytic properties.