Zinc‐based sorbents with ordered mesoporous structure were modified with aluminium and the key factors in the preparation were optimized based on the results of desulphurization tests performed in a fixed‐bed reactor with simulated coal gas. It was shown that the sorbents for hydrogen sulphide removal reached an optimum sulphur capacity of 9.14% when prepared under conditions of 10.0 crystalline pH, 30:1 Si:Al molar ratio, 0.32:1 Zn:Si molar ratio, and 1:3 Zn:TAA molar ratio. The sorbent without aluminium was synthesized synchronously as a comparison sample to investigate the effect of aluminium addition on the desulphurization properties. The surface acidity of the sorbents is enhanced by the addition of aluminium, and the sulphur capacity of the aluminium‐doped sorbent is consequently lower compared to that of aluminium‐free sorbent. Nevertheless, the aluminium‐doped sorbent shows a significant advantage in stability of performance over multiple desulphurization–regeneration cycles and reaches an 81% retention rate of sulphur capacity after five desulphurization, while the aluminium‐free sorbent is only 51% in contrast. The characterization results manifest that aluminium enters the carrier skeleton and increases the wall thickness, which alleviates the collapse of the carrier pore channels and the agglomeration of the active components during the desulphurization process. Stable pore structures and highly dispersed active components facilitate the mass transfer in the reaction process after multiple desulphurization. As a result, the aluminium‐doped sorbent exhibits better performance stability in high temperature coal gas desulphurization.