This paper proposes a hybrid heuristic and criteria-based method of optimum design which combines the advantages of both the iterated simulated annealing (SA) algorithm and the rigorously derived optimality criteria (OC) for structural optimum design of reinforced concrete (RC) buildings under multi-load cases based on the current Chinese design codes. The entire optimum design procedure is divided into two parts: strength optimum design and stiffness optimum design. A modified SA with the strategy of adaptive feasible region is proposed to perform the discrete optimization of RC frame structures under the strength constraints. The optimum stiffness design is conducted using OC method with the optimum results of strength optimum design as the lower bounds of member size. The proposed method is integrated into the commercial software packages for building structural design, SATWE, and for finite element analysis, ANSYS, for practical applications. Finally, two practical frame-shear-wall structures (15-story and 30-story) are optimized to illustrate the effectiveness and practicality of the proposed optimum design method.