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Metal halide perovskite semiconductors poses attractive light-harvesting and charge carrier transport properties for photovoltaics, however perovskite solar cells (PSCs) lack sufficient device stability for industrial up-scaling and real-world deployment. Throughout the natural world, highly durable biomaterials offer intriguing design inspiration which should be leveraged for improved PSC performance. In this Review, at the molecular level, we elaborate on nature-inspired molecular interactions for crystallization control and degradation prevention, such as natural biopolymers, starchpolyiodide coordinated compounds, that can reduce operational degradation by 11% over 1470 hours. At the microstructural level, we summarize nature-inspired strategies to foster self-healing and improved mechanical properties of PSCs. At the device level, we explore nature-inspired macroscopic functionalities for systematically controlling light management, heat transport, and encapsulation in PSCs, such as moth-eye inspired structures that can improve both efficiency by ~3% and shelf-stability over 5000 hours. We envision that drawing inspiration from nature's diverse resources could revolutionize PSC research and the clean energy landscape beyond photovoltaics by utilizing biomolecular multifunctional interactions, improving efficiency and lifetime, along with low cost (