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Despite possessing versatile properties and great potential for biomedical research, the number of studies on the application of polydopamine-functionalized gold nanoparticles (Au@PDA NPs) remains infrequent due to their preparation procedure, which consists of multiple-steps employing hazardous redox agents. We herein present an unprecedented single-step synthesis protocol using a non-equilibrium atmospheric pressure plasma jet to trigger the redox reaction between dopamine (DA) and gold ions in distilled water to simplify the fabrication process, eliminating the use of additional chemicals. Under the plasma treatment, the solvated electrons and reactive oxygen species generated from the plasma–liquid interaction can simultaneously reduce Au ions to metallic Au and oxidize DA to polydopamine (PDA), respectively, thus leading to the formation of Au@PDA NPs. The simultaneous reactions between …