Coconut-shell-based activated carbon (ACS-1) was used as a sorbent to simultaneously remove H2S and SO2 from simulated Claus tail gas. Adsorption and regeneration tests were performed to systematically investigate the desulfurization performance, regenerability, and stability of the ACS-1 sorbent. The physicochemical properties of ACS-1 before and after adsorption were characterized by nitrogen adsorption, scanning electron microscopy, energy-dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy. The experimental results revealed that the ACS-1 sorbent exhibited good desulfurization performance under a feed gas of H2S (20 000 ppmv), SO2 (10 000 ppmv), and N2 (balance), and the concentrations of H2S and SO2 in the simulated Claus tail gas could be reduced to less than 10 mg/m3 by ACS-1. The breakthrough sulfur capacity of ACS-1 is 64.27 mg of S/g of sorbent at an adsorption temperature of 30 °C and a gas hourly space velocity of 237.7 h–1. The micropores with sizes of around 0.5 nm in ACS-1 a...