The air-supported membrane coal shed is widely used in bulk cargo terminals. It not only effectively protects goods from adverse weather conditions but also helps reduce coal dust and harmful gas emissions, promoting the green and sustainable development of ports. However, in practical engineering, the design parameters of the coal shed are often based on experience, making it difficult to accurately assess the quality of the structural design. The flexibility of the membrane material also makes the structure susceptible to deformation or tearing. This paper mainly focuses on modeling and solving the optimization design issues of air-supported membrane coal shed structures. According to the evaluation criteria for the form of air-supported membrane coal sheds, a multi-objective structural optimization model is established to minimize the maximum stress on the membrane surface, ensure uniform stress distribution, maximize structural stiffness, and minimize costs. The study utilizes a combined optimization approach using ANSYS 19.0 and MATLAB 2016a, incorporating an improved NSGA-II algorithm program developed in MATLAB into ANSYS for structural form analysis and load calculation. The research results indicate that the optimal solution reduces the maximum stress on the loaded membrane surface by 5.36%, shortens the maximum displacement by 30.3%, and saves on economic costs by 9.85%. Compared to traditional empirical design methods, the joint use of MATLAB and ANSYS for optimization design can provide more superior solutions, helping ports to achieve environmental protection and economic efficiency goals.