Control of high-rise structures under seismic excitations was investigated using a passive hybrid control system consisting of a base-isolation (BI) subsystem and a passive tuned liquid column damper (TLCD) system. Both of the systems were optimized considering using the other system in the same structure. An optimization method was developed, and a computer code was written based on dynamic analysis of the structure and metaheuristic optimization methods. Within the scope of the study, a general solution was found by using many earthquake records during the optimization process. Moreover, one of the most suitable and successful metaheuristic algorithms was used in this study. In addition, numerical simulations were performed on a benchmark high-rise building structure to investigate the effectiveness of the optimized hybrid control system in controlling the seismic response of the building. The performance of the base-isolated TLCD-controlled structure was examined when the TLCD was placed on the base floor by using a set of 44 recorded ground motions as base excitations. Based on the results obtained from this study, the use of a base-isolation subsystem decoupling the superstructure from the ground motions by lowering the structure’s fundamental natural frequency reduces the structural responses of the building in most cases. The responses of the base-isolation subsystem were not too large since the parameters of the BI subsystem were optimized specifically for the investigated structure. Nevertheless, displacements of BI might exceed the maximum limit to undesirable values in some cases. The TLCD system appears to be quite effective in protecting the base-isolation subsystem by reducing its displacements to the maximum allowable limit or below when attached to it. Moreover, the proposed passive hybrid control system can effectively reduce the structural responses under seismic excitations.