Waste adsorbents generated from treating Cr(VI)-containing wastewater are hazardous materials and generally landfilled or treated by acid or base desorption, with concomitant high cost and toxic effects. The present work shows that these Cr adsorbents can be reused as highly efficient catalysts for treating sulfur-containing VOCs (CH3SH), not only avoiding the economic and environmental impact from the conventional approaches, but also achieving the efficient treatment of sulfur-containing waste gas. Importantly, these reused Cr adsorbents exhibit enhanced activity and stability compared with the catalysts reported elsewhere, indicating a new avenue of green chemistry. The highly toxic adsorbed Cr(VI) species are reduced to a Cr2O3 crystalline phase by calcination and finally immobilized as a Cr2S3 solid phase while converting and eliminating CH3SH. Still, the presence of Cr(VI) species on the reused Cr adsorbent provides enough reactive sites for reaction, but high concentration of Cr(VI) species causes serious accumulation of coke deposit on the catalyst, leading to fast deactivation of the catalyst.