Scalable Nondestructive Exfoliation of Layered Materials Into Monolayers via Shear‐Transducing Interfaces

ABSTRACT Mechanochemical exfoliation via ball milling holds great promise for scalable production of two‐dimensional (2D) materials, but it is fundamentally hindered by impact‐induced fragmentation and thermo‐oxidative degradation during high‐energy milling. Herein, we report a shear‐dominated exfoliation (SDE) strategy using viscoelastic green polymer as an active energy regulator that redirects destructive impact into beneficial shear. This enables the construction of a shear‐conducting interface, promoting interlayer delamination, suppressing chaotic fragmentation, and achieving in situ thermal‐oxidation protection. The SDE approach achieves hundred‐gram‐scale monolayer fluorinated graphene (FGr) with well‐preserved fluorine integrity, and demonstrates broad universality for diverse layered materials. Remarkably, the FGr affords high‐rate energy densities in 25 Ah Li/CF x cells (832.0 Wh kg −1 at 0.1 C; 737.5 Wh kg −1 at 0.5 C). Meanwhile, the unoxidized monolayer MXene and black phosphorus demonstrate excellent electromagnetic interference shielding and superior rate capability for Li + storage. Our work bridges scalability, integrity, and green chemistry for industrial manufacturing of 2D materials.