Building structures are considered as major contributors to global energy consumption (30–40%) and are responsible for 40–50% of greenhouse gas emissions. Due to their high energy consumption and material use, tall buildings have drawn particular attention with respect to their environmental impact. The influence of structural systems on the environmental performance of tall buildings is studied in this work, through calculating the embodied energy and CO2 emissions of construction materials. In this direction, characteristic structural systems of tall buildings are considered in order to compare their environmental behaviour and account for their differences on the amount of construction materials used for their formation. In order to achieve this comparison, the structural systems are material-cost optimized using an optimization computing platform (OCP) developed by the authors for solving real-world structural design optimization problems. The results of this research provide valuable findings for the significant role of structural optimization in sustainable design of tall buildings as well as in limiting the use of construction materials.