Flexible intelligent materials are desired to effectively regulate their own deformation and accurately sense their immediate morphology at the same time. Graphene foam is an attractive material for strain sensing and electrical/thermal performance control due to its outstanding mechanical, electrical, and thermal properties. However, graphene‐foam‐based materials with both strain sensing and deformation control capabilities are rarely reported. Here, a multiscale design of graphene foam with a single‐layer‐graphene‐dominated microstructure and resilient 3D network architecture, which leads to exceptional strain sensing performance as well as modulation ability of the electrical and thermal conductivity for shape memory polymers, is reported. The graphene foams exhibit a strain detection limit of 0.033%, a rapid response of 53 ms, long‐term stability over 10 000 cycles, significant thermoacoustic effect, and great heat‐generation and heat‐diffusion ability. By combining these advantages, an electro‐activated shape‐memory composite that is capable of monitoring its own shape state during its morphing process, is demonstrated.

The advancements in the development of intelligent systems have resulted in an increase in the number, density, and distribution range of sensors. Traditional energy supply methods cannot meet the demands of the complex and variable sensor systems. However, the emergence of self-powered sensing devices that generate energy from their surroundings has provided a solution to this problem. Graphene, which has both an excellent sensing performance and wide range of applications in energy devices, facilitates the design of self-powered sensing systems. In recent years, several graphene-based self-powered sensors have been developed to overcome the design limitations of sensing systems. In this review, these sensors are divided into five categories according to their different energy conversion methods.(1) Self-powered by the electrochemical effect. The traditional electrochemical battery can be designed as a flexible structure that is responsive to external stimuli, including pressure, deformation, humidity, light, and temperature. It is an effective, stable, self-driving sensor, with working life determined by the amount of oxidizing/reducing agent present and the reaction rate. Flexible electrochemical cells with a high strain sensitivity ((I/I0)/ε = 124) and stretchability (2000%) have been achieved. (2) Self-powered by the photovoltaic effect. Graphene can form a Schottky junction when coupled with various semiconducting materials, such as Si, GaAs, MoS2, and some of their nanostructures. In these heterostructures, the van der Waals interface exhibits a Schottky barrier, which can separate photogenerated electron-hole pairs without external bias. Graphene-based Schottky junctions have been widely used as self-powered photodetectors with extremely high responsivities ( ~149 A•W −1 ). (3) Self-powered by the triboelectric effect. The contact and separation of two surfaces can result in the separation of charges due to the difference in electron affinities of the materials. This results in an induced electrostatic force between the electrodes, thereby driving the flow of electrons in an external circuit. Triboelectric nanogenerators can realize self-driving touch/pressure sensing and are used for several applications, including touch screens, neural finger skin, and electronic skin. (4) Self-powered by the hydrovoltaic effect. Graphene can interact with water at the solid-liquid interface and generate an electrical signal. Therefore, graphene-based hydrovoltaic devices can constitute very simple self-driving sensors that are efficient in determining fluid flow, solution concentration, and humidity, among others. (5) Self-powered by other effects, such as the thermoelectric effect, piezoelectric effect, or pyroelectric effect. Although the electrical signals generated by these effects are relatively weak, they can be used for some special applications, such as temperature or infrared sensors. Finally, we discuss the future developments, challenges, and prospects of graphene-based self-powered sensing devices and syste...

Shape memory polymers (SMPs) have gained increasing attention as intelligent morphing materials. However, due to the inherent electrical insulation and poor thermal conductivity of polymers, deformation and temperature control of SMPs usually require external heating devices, bringing about design inconveniences and fragility of interfaces. Herein, we report a shape memory composite that integrates reliable temperature and shape control functions into the interior. The composite is comprised of resin-based SMP and three-dimensional interconnected graphene foam (3DGF), exhibiting a high recovery rate and thermal/electrical conductivity. With only 0.26 wt% of graphene foam, the composite can improve electrical conductivity by 15 orders of magnitude, thermal conductivity by 180%, tensile strength by 64.8%, and shape recovery speed by 154%. Using a very simple Joule heating scheme, decimeter-sized samples of the composite deformed to their preset shapes in less than 10 s.