In recent years, actuators based on carbon nanotube (CNT) or graphene demonstrate great potential applications in the fields of artificial muscles, smart switches, robotics, and so on. The electrothermal and photothermal bending actuators based on CNT/graphene and polymer composites show large bending actuations, which are superior to traditional thermaldriven actuators. However, the influence of material parameters (thickness, temperature change, etc.) on the actuation performance needs to be further studied, because it is a critical point to the design and fabrication of high-performance actuators. In this work, finite element analysis (FEA) is employed to simulate the actuation performance of CNT/polymer actuator, which has a bilayer structure. The main focus of this work is to design and to optimize material parameters by using computational method. FEA simulation results show that each layer thickness of actuator has an important influence on the actuation deformation. A maximum curvature of 2.7 cm −1 is obtained by simulation, which is much larger than most of the actuator curvature reported in previous experiments. What is more, larger temperature change and larger difference of coefficient of thermal expansion (CTE) between two layers will result in larger bending actuation. This study is expected to provide valuable theoretical reference for the design and realization of CNT-based thermal actuator with ultra-large actuation performance.