Developing efficient, sustainable, and biocompatible high‐tech nanoplatforms derived from naturally existing components in living organisms is highly beneficial for diverse advanced biomedical applications. Melanins are nontoxic natural biopolymers owning widespread distribution in various biosystems, possessing fascinating physicochemical properties and playing significant physiological roles. The multifunctionality together with intrinsic biocompatibility renders bioinspired melanin‐like nanomaterials considerably promising as a versatile and powerful nanoplatform with broad bioapplication prospects. This panoramic Review starts with an overview of the fundamental physicochemical properties, preparation methods, and polymerization mechanisms of melanins. A systematical and well‐bedded description of recent advancements of melanin‐like nanomaterials regarding diverse biomedical applications is then given, mainly focusing on biological imaging, photothermal therapy, drug delivery for tumor treatment, and other emerging biomedicine‐related implementations. Finally, current challenges toward clinical translation with an emphasis on innovative design strategies and future striving directions are rationally discussed. This comprehensive and detailed Review provides a deep understanding of the current research status of melanin‐like nanomaterials and is expected to motivate further optimization of the design of novel tailorable and marketable multifunctional nanoplatforms in biomedicine.

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