Wood-based materials are attracting extensive attention for applications in energy storage due to their environmental friendliness and the presence of numerous channels in their structure. However, the poor conductivity and flexibility of wood restrict its application. Although some researchers have made several efforts to improve the conductivity of wood by carbonization, the wood-based materials become brittle instead of flexible. Moreover, the cycling stability of carbonized wood-based materials becomes very poor due to their falling off during the process of electrochemical energy storage. Herein, for the first time, a smart carbonized lignin-free wood (CLFW)@Ni–NiS/vitrimer(V) composite multifunctional material with good reshaping, shape-memory, and self-healing properties was designed and fabricated. When assembled to a symmetric supercapacitor, the resultant CLFW@Ni–NiS/V hybrid showed not only the high gravimetric, areal, and volumetric energy densities of 38 W h kg⁻¹, 687 μW h cm⁻², and 58 W h L⁻¹ and simultaneously maintained the high power densities of 56 kW kg⁻¹, 202 mW cm⁻², and 39 kW L⁻¹, but also significantly enhanced cycling stability, respectively. In addition, CLFW@Ni–NiS/V presented good ORR and strain sensor properties. These outstanding advantages highlight the huge potential of smart wood-based materials with variable, shape-memory, and self-healing properties for applications in supercapacitors, catalysts, and sensors.

Recently, with the continuous development of human society and the continuous innovation of technologies, the intelligence era has arrived. Various intelligent electronic devices continue to be developed, in which flexible wearable electronic devices are highly favored by people. To meet the requirements of the normal operation of intelligent devices, the key point lies in the development of new smart energy storage devices. Accordingly, smart supercapacitors have been widely focused on and studied by researchers recently with the introduction of intelligent functions, such as electrochromism, self‐healing, and shape memory, into supercapacitors to broaden their application fields and promote their smart development. This can meet not only people's energy needs but also people's diverse personality needs and make our life more convenient, fast, and more intelligent than ever. Therefore, it is very important to summarize related work on smart supercapacitors. Although researchers have performed much research on smart supercapacitors, there is still little literature summary on the related work of different smart supercapacitors. Accordingly, this paper mainly introduces the research progress on electrochromic, self‐healing, shape memory, and self‐charging smart supercapacitors in recent years and discusses the development prospects and challenges of smart supercapacitors.