Smart wearable devices have demonstrated promising applications in virtual reality, health monitoring, motion tracking, and beyond. Recently, MXene with fascinating physical/ chemical properties has been considered an ideal candidate to make the core components of smart wearable devices such as soft actuators and sensors. However, most current MXene-based devices present only actuating or sensing features, which may prohibit the integrated development of smart wearable devices. Here, a multifunctional MXene/tape bilayer film that integrates multiresponsive actuating and sensing functions is reported. Owing to the distinct hygroexpansion effect and thermal expansivity of two layers, the MXene/tape bilayer film can be manipulated under moisture, light, and electricity. Meanwhile, this MXene/tape bilayer film can be used as a strain sensor by introducing microcracks into the MXene layer. As a proof of concept, smart devices, including a wearable interactive manipulator system and a wearable interactive gripper system, are fabricated, revealing great potential for developing flexible robotics and smart wearable devices.