Perovskite solar cells (PeSCs) have been considered as one of the most promising photovoltaic technologies due to their high efficiency, low-cost and facile fabrication process. The power conversion efficiency and stability of PeSCs highly depend on the quality of perovskite film and the interfaces in the device, which are the main sources of PeSCs nonradiative recombination losses. Natural biomaterials, with the advantages of earth-abundance, non-toxicity, and biocompatibility, have shown huge potential to improve both perovskite layer and interfaces in PeSCs. Herein, the latest progress using natural biomaterials to achieve high-performance PeSCs is reviewed. It’s discussed the roles of natural biomaterials on perovskite film in terms of morphology optimization, defect passivation and energetics modification. Meanwhile, the strategies using natural biomaterials to create superior interface between perovskite and charge transport layer, and to build stretchable, biocompatible, and biodegradable electrodes are present. Finally, an outlook on the further development of PeSCs with respect to natural biomaterials is provided.