Continuous MXene/graphene fibers are fabricatedviawet-spinning assembly strategy, from which fiber-constructed supercapacitors are obtained that exhibit both high capacitance and flexibility.

Carbon aerogels demonstrate wide applications for their ultralow density, rich porosity, and multifunctionalities. Their compressive elasticity has been achieved by different carbons. However, reversibly high stretchability of neat carbon aerogels is still a great challenge owing to their extremely dilute brittle interconnections and poorly ductile cells. Here we report highly stretchable neat carbon aerogels with a retractable 200% elongation through hierarchical synergistic assembly. The hierarchical buckled structures and synergistic reinforcement between graphene and carbon nanotubes enable a temperature-invariable, recoverable stretching elasticity with small energy dissipation (~0.1, 100% strain) and high fatigue resistance more than 106 cycles. The ultralight carbon aerogels with both stretchability and compressibility were designed as strain sensors for logic identification of sophisticated shape conversions. Our methodology paves the way to highly stretchable carbon and neat inorganic materials with extensive applications in aerospace, smart robots, and wearable devices.

Graphene fiber (GF) is a macroscopically assembled fibrous material made of individual units of graphene and its derivatives. Beyond traditional carbon fibers, graphene building blocks consisting of regulable sizes and regular orientations of GF are expected to generate extreme mechanical and transport properties, as well as multiple functions in smart electronic fibrous devices and textiles. Here, the features of GF are presented along four lines: preparation, morphology, structure–performance correlations, and state‐of‐the‐art applications as flexible and wearable electronics. The principles, experiments, and keys of fabricating GF from graphite with different methods, focusing on the industrially viable mainstream strategy, wet spinning, are introduced. Then, the fundamental relationship between the mechanical and transport properties and the structure, including both highly condensed structures for high‐performance and hierarchical structures for multiple functions, is presented. The advances of GF based on structure–performance formulas boost its functional applications, especially in electronic devices. Finally, the possible promotion methods and structural–functional integrated applications of GF are discussed.

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