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The development of green, controllable, and simplified pathways for rapid dopamine polymerization holds significant importance in the field of polydopamine (PDA) surface chemistry. In this study, a green strategy is successfully devised to accelerate and control the polymerization of dopamine through the introduction of ozone (O3). The findings reveal that ozone serves as an eco‐friendly trigger, significantly accelerating the dopamine polymerization process across a broad pH range, spanning from 4.0 to 10.0. Notably, the deposition rate of PDA coatings on a silicon wafer reaches an impressive value of ≈64.8 nm h−1 (pH 8.5), which is 30 times higher than that of traditional air‐assisted PDA and comparable to the fastest reported method. Furthermore, ozone exhibits the ability to accelerate dopamine polymerization even under low temperatures. It also enables control over the inhibition–initiation of the polymerization process by regulating the "ON/OFF" mode of the ozone gas. Moreover, the ozone‐induced PDA coatings demonstrate exceptional characteristics, including high homogeneity, good hydrophilicity, and remarkable chemical and mechanical stability. Additionally, the ozone‐induced PDA coatings can be rapidly and effectively deposited onto a wide range of substrates, particularly those that are adhesion‐resistant, such as polytetrafluoroethylene (PTFE). [ABSTRACT FROM AUTHOR]