Synthetic Multifunctional Graphene Composites with Reshaping and Self‐Healing Features via a Facile Biomineralization‐Inspired Process

Since graphene is a type of 2D carbon material with excellent mechanical, electrical, thermal, and optical properties, the efficient preparation of graphene macroscopic assemblies is significant in the potentially large‐scale application of graphene sheets. Conventional preparation methods of graphene macroscopic assemblies need strict conditions, and, once formed, the assemblies cannot be edited, reshaped, or recycled. Herein, inspired by the biomineralization process, a feasible approach of shapeable, multimanipulatable, and recyclable gel‐like composite consisting of graphene oxide/poly(acrylic acid)/amorphous calcium carbonate (GO‐PAA‐ACC) is designed. This GO‐PAA‐ACC material can be facilely synthesized at room temperature with a cross‐linking network structure formed during the preparation process. Remarkably, it is stretchable, malleable, self‐healable, and easy to process in the wet state, but tough and rigid in the dried state. In addition, these two states can be readily switched by adjusting the water content, which shows recyclability and can be used for 3D printing to form varied architectures. Furthermore, GO‐PAA‐ACC can be functionalized or processed to meet a variety of specific application requirements (e.g., energy‐storage, actuators). The preparation method of GO‐PAA‐ACC composite in this work also provides a novel strategy for the versatile macroscopic assembly of other materials, which is low‐cost, efficient, and convenient for broad application.