In this work, we have successfully prepared core–shell nanoparticles (Fe₃O₄@PDA) wrapped with Ag using a simple and green synthesis method. Without an external reducing agent, silver nanoparticles (Ag NPs) with good dispersibility were directly reduced and deposited on a polydopamine (PDA) layer. Fe₃O₄@PDA@Ag showed excellent catalytic activity and recyclability for 4-nitrophenol, and also exhibited good catalytic selectivity for organic dyes (MO and MB). This simple and green synthesis method will provide a platform for other catalytic applications.