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Removal of highly toxic H₂S for pollution control and operational safety is a pressing need. For this purpose, a montmorillonite intercalated with Cu(II)-phenanthroline complex [Cu[(Phen)(H₂O)₂]²⁺ (Mt-CuPhen) was prepared to capture gaseous H₂S under mild conditions. This hybrid material was simple to obtain and demonstrated an outstanding ability to entrap H₂S at room temperature, retaining high efficiency for a very long time (up to 36.8 g of S/100 g Mt-CuPhen after 3 months of exposure). Sorbent and H₂S uptake were investigated by elemental analysis, X-ray powder diffraction measurements, diffuse reflectance (DR) UV–Vis and infrared spectroscopy, thermal analysis and evolved gas mass spectrometry, scanning electron microscopy equipped with energy-dispersive X-ray spectrometer, and X-ray absorption spectroscopy. The H₂S capture was studied over time and a mechanism of action was proposed. The entrapping involves a catalytic mechanism in which [Cu[(Phen)(H₂O)₂]²⁺ acts as catalyst for H₂S oxidation to S⁰ by atmospheric oxygen. The low cost and the long-lasting performance for H₂S removal render Mt-CuPhen an extremely appealing trap for H₂S removal and a promising material for many technological applications.