Polydopamine (PDA) is a major type of artificial melanin material with many interesting properties such as antioxidant activity, free‐radical scavenging, high photothermal conversion efficiency, and strong metal‐ion chelation. The high affinity of PDA to a wide range of metals/metal ions has offered a new class of functional metal‐containing polydopamine (MPDA) nanomaterials with promising functions and extensive applications. Understanding and controlling the metal coordination environment is vital to achieve desirable functions for which such materials can be exploited. MPDA nanomaterials with metal/metal ions as the active functions are reviewed, including their synthesis and metal coordination environment and their applications in catalysis, batteries, solar cells, capacitors, medical imaging, cancer therapy, antifouling, and antibacterial coating. The current trends, limitations, and future directions of this area are also explored.