The remarkable functionality of biological systems in detecting and adapting to various environmental conditions has inspired the design of the latest electronics and robots with advanced features. This review focuses on intelligent bio-inspired strategies for developing soft bioelectronics and robotics that can accommodate nanocomposite adhesives and integrate them into biological surfaces. The underlying principles of the material and structural design of nanocomposite adhesives were investigated for practical applications with excellent functionalities, such as soft skin-attachable health care sensors, highly stretchable adhesive electrodes, switchable adhesion, and untethered soft robotics. In addition, we have discussed recent progress in the development of effective fabrication methods for micro/nanostructures for integration into devices, presenting the current challenges and prospects.