A combination between the nanostructured photocatalyst and cellulose-based materials promotes a new functionality of cellulose towards the development of new bio-hybrid materials for water treatment and renewable energy applications. In this study, nanocellulose (CNC) was synthesized from sugarcane bagasse (SCB) biomass via formic /peroxyformic acid process treatment and acid hydrolysis at an atmospheric pressure. The resulting CNC of sugarcane bagasse were characterized by crystallinity index, chemical structure and morphology. X-ray diffraction (XRD) analysis revealed that the crystallinity increased with successive treatments. Images generated by TEM showed that CNC was rod-like in morphology, average diameter and length of 10 nm and 410 nm, respectively. The obtained CNC was used as a biotemplate for the synthesis of copper oxide (CuO) nanostructures through in - situ solution casting method. The photo-Fenton catalytic activity was evaluated via the degradation of methylene blue under sunlight irradiation with H2O2 as a oxidizing agent. The methylene blue degradation ratio of CuO/ CNC composite could achieve 98% in 150 min. The addition of H2O2 enhanced photocatalytic activities of the CuO/CNC. H2O2 not only prevented the recombination of charge carriers by accepting the photogenerated electrons and holes effectively but also produced additional OH.