The tall desulphurization tower belongs to the thin-wall steel structure with round section, which has the characteristics of large flexibility, small damping and abrupt change of upper section. Under wind load, the tower is prone to severe vibration in along-wind and across-wind directions. In order to realize efficient and lightweight control of the wind-induced vibration of the tower, a tuned mass inerter system (TMIS) isadopted in this study. Based on the derived frequency response function formula of the desulfurization tower-TMIS coupling system, theoptimal design method of the TMIS forboth along-wind and across-wind induced vibration control of the toweris established. Finally, the vibration control performance of TMIS on the tower is compared with that of traditional tuned mass damper (TMD) and tuned mass inerter damper (TMDI). The results show that the TMIS optimized with the frequency domain response and H∞ norm as targets has excellent control performance on vibration mitigation of the tower in both along-wind and across-wind directions.Moreover, the TMIS demonstrates better lightweight effect on vibration control in across-wind direction than that in along-wind direction, and its control performance is superior overthat of the TMD and TMDI.