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This paper addresses the effective use of carbon fiber reinforced polymeric (CFRP) materials in the cable system. As the span length of cable-stayed bridges increases, several technical challenges become more dominant with traditional material. This paper mainly focuses on improving the aerodynamic performance through implementing CFRP composites in the cable system in combination with steel. In order to maximize the improvement, a genetic algorithm (GA)-based optimization procedure is developed to optimize the distribution of CFRP and steel. A numerical example is presented and the results suggest the typical composition of an optimized CFRP-steel cable system for long-span cable-stayed bridges.