The challenging post-surgery management of bone metastasis sees the needs for multi-functional bone scaffolds that offer multi-modal therapeutic functions. Through a nature-inspired layer-by-layer assembly process, we developed a unique multi-functional tissue scaffold that consists of porous polyurethane substrate and nanoscale chitosan/ graphene oxide hybrid coating. Alternative layers of drug laden chitosan and graphene oxide nanosheets were held together through strong electrostatic interaction, giving rise to a robust multilayer architecture with control over structural element orientation and chemical composition at nanoscale. For the first time, proof-of-concept on combining pH-controlled co-delivery of multiple therapeutic agents and photothermal therapy have demonstrated, in the context of malignant bone cancer treatment. Our scaffold system can be tailored to the patient’s specific needs through loading of bespoke therapeutic agents and offering on-demand photothermal therapy. The methodology can also be generalized to create functional surfaces for a wide range of biomedical devices as well as for applications beyond healthcare technology.