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Intercalated layered materials offer distinctive properties and serve as precursors for important two-dimensional (2D) materials. However, intercalation of non–van der Waals structures, which can expand the family of 2D materials, is difficult. We report a structural editing protocol for layered carbides (MAX phases) and their 2D derivatives (MXenes). Gap-opening and species-intercalating stages were respectively mediated by chemical scissors and intercalants, which created a large family of MAX phases with unconventional elements and structures, as well as MXenes with versatile terminals. The removal of terminals in MXenes with metal scissors and then the stitching of 2D carbide nanosheets with atom intercalation leads to the reconstruction of MAX phases and a family of metal-intercalated 2D carbides, both of which may drive advances in fields ranging from energy to printed electronics. 

Abstract Electrode stabilization by surface passivation has been explored as the most crucial step to develop long‐cycle lithium‐ion batteries (LIBs). In this work, functionally graded materials consisting of “conversion‐type” iron‐doped nickel oxyfluoride (NiFeOF) cathode covered with a homologous passivation layer (HPL) are rationally designed for long‐cycle LIBs. The compact and fluorine‐rich HPL plays dual roles in suppressing the volume change of NiFeOF porous cathode and minimizing the dissolution of transition metals during LIBs cycling by forming a structure/composition gradient. The structure and composition of HPL reconstructs during lithiation/delithiation, buffering the volume change and trapping the dissolved transition metals. As a result, a high capacity of 175 mAh g⁻¹(equal to an outstanding volumetric capacity of 936 Ah L⁻¹) with a greatly reduced capacity decay rate of 0.012% per cycle for 1000 cycles is achieved, which is superior to the NiFeOF porous film without HPL and commercially available NiF₂‐FeF₃powders. The proposed chemical and structure reconstruction mechanism of HPL opens a new avenue for the novel materials development for long‐cycle LIBs.