The preparation of a Cu-based sorbent supported by cost-effective AlOOH is proposed. A Cu-based sorbent for thiophene removal from coke oven gas was synthesized via coprecipitation, and the effect of AlOOH addition on the dispersion of activated Cu species and desulfurization properties was investigated. At an AlOOH content of 25%, smaller and more highly dispersed Cu grains, along with ZnO crystalline phases, were present on the surface of the Cu-based sorbent. The enhanced Cu-ZnO interaction contributed to the superior desulfurization performance (Q b-thiophene = 30.43 mg/g). The incorporation of an appropriate amount of AlOOH into the binary system during synthesis produces a highly active sorbent with superior Cu dispersion and smaller Cu grains, thereby fulfilling the requirements of industrial applications at a lower production cost.