In comparison to the traditional fixed-angle trajectory, the variable-angle trajectory has a greater design space. However, it is a challenge to determine which common design curve structure is the most effective for improving mechanical performance. This work explores the effects of various design curves such as fixed-angle curve, linear curve, arc curve, sine curve, Bezier curve, and cubic polynomial curve trajectories on mechanical performance of laminates, including vibration modal performance and buckling performance. Genetic algorithm and improved NSGA-II algorithm are then used to optimize various curve structures. The results are confirmed utilizing thermoplastic Carbon Fiber (CF)/Polyether-Ether-Ketone (PEEK) laminates made by robotic fiber placement experiments. The relationship model between different mechanical performance and curve design variables is established. The optimization of variable-angle structure with mechanical properties as input variables is achieved. Meanwhile, a full-process angle-variable laying software platform from trajectory planning (CAD), trajectory optimization to manufacturing (CAM) is developed for facilitating the fiber placement application.