Currently, tremendous efforts are being devoted to develop high-performance electrochemical energy-storage materials and devices. Conventional electrochemical energy-storage systems are confronted with great challenges to achieve high energy density, long cycle-life, excellent biocompatibility and environmental friendliness. The biological energy metabolism and storage systems have appealing merits of high efficiency, sophisticated regulation, clean and renewability, and the rational design and fabrication of advanced electrochemical energy-storage materials and smart devices inspired by nature have made some breakthrough progresses, recently. In this review, we summarize the latest developments in the field of nature-inspired electrochemical energy-storage materials and devices. Specifically, the nature-inspired exploration, preparation and modification of electrochemical energy-storage related materials including the active materials, binders, and separators are introduced. Furthermore, nature-inspired design and fabrication of smart energy-storage devices such as self-healing supercapacitors, supercapacitors with ultrahigh operating voltage, and self-rechargeable batteries are also discussed. The review aims to provide insights and expanded research perspectives for further study in this exciting field based on our comprehensive discussions.