Synthetic melanin is a mimic of natural melanin analogue with intriguing properties such as metal−ion chelation, redox activity, adhesion, and broadband absorption. Melanin-inspired composite materials are formulated by assembly of melanin with other types of inorganic and organic components to target, combine, and build up the functionality, far beyond their natural capabilities. Developing efficient and universal methodologies to prepare melaninbased composite materials with unique functionality is vital for their further applications. In this review, we summarize three types of synthetic approaches, predoping, surface engineering, and physical blending, to access various melanin-inspired composite materials with distinctive structure and properties. The applications of melanininspired composite materials in free radical scavenging, bioimaging, antifouling, and catalytic applications are also reviewed. This review also concludes current challenges that must be addressed and research opportunities in future studies.