High‐Yield Exfoliation of Large MXene with Flake Sizes over 10 µm Using Edge‐Anchored Carbon Nanotubes

Abstract The exceptional properties of 2D transition metal carbides and nitrides (MXene) have led to numerous promising applications. However, the performance of MXene is often dependent on the size of the flakes, and obtaining large‐sized, high‐quality MXene flakes remains challenging. Herein, a carbon nanotube (CNT)‐assisted exfoliation strategy is introduced, which significantly improves the yield of large‐flake MXene while entirely transforming the centrifugation residues into small‐flake MXene, resulting in waste‐free synthesis of MXene. The average size of the obtained MXene flakes can reach over 10 and 0.7 µm for the two populations, respectively. Additionally, the capacitive performance of MXene can be greatly enhanced with a small amount of CNTs. As a proof of concept, a planar interdigital micro‐supercapacitor with heterogeneous layers assembled by large‐ and small‐flake MXene simultaneously exhibits outstanding synergistic enhancement in volumetric capacitance (1072 F cm⁻ 3 ) and energy density (53.5 mWh cm⁻ 3 ). This CNT‐assisted method provides explicit directions for achieving the ideal utilization of MXene, improving the yield of large flakes while making judicious use of waste, to meet specific application needs.