Synthetic Pathways in Mg‐Al‐based LDH Systems to a Versatile Library of Single‐layer Porous Derivatives With Structural Transformations and Tunable Doping

ABSTRACT Layered double hydroxides (LDHs) are versatile 2D materials with highly tunable compositions and structures. However, existing strategies typically rely on composition‐specific or phase‐limited transformations, making the controlled construction of single‐layer porous layered nanomaterials with diverse chemical matrices highly challenging. Therefore, the development of a general strategy for single‐layer porous LDH‐derived materials remains elusive. Here, we report a general and versatile synthetic framework in Mg‐Al‐based LDH systems that enables the controlled construction of single‐layer porous layered nanomaterials with distinct chemical matrices derived from a common LDH precursor and tunable doping. Using Nd as a representative doping model, the systematic transformation from LDH to layered double oxides (LDO), layered double fluorides (LDF), and layered double oxysulfides (LDOS) was achieved while preserving an ultrathin porous 2D morphology. The generality of this approach was further demonstrated by extending the strategy to other dopant elements, spanning rare‐earth and transition‐metal systems. This unified platform allowed systematic correlation of matrix chemistry with functionality, including enhanced luminescence in rare‐earth‐doped fluorides, high magnetic relaxivity in porous oxides, and tunable band structures in transition‐metal‐doped oxysulfides. This work, therefore, established a general and versatile paradigm for designing multifunctional LDH‐derived porous 2D materials.