Layered double hydroxides (LDHs) are ac lass of 2D anionic materials exhibiting wide chemical versatility and promising applications in different fields, ranging from catalysis to energy storage and conversion.H owever,t he covalent chemistry of this kind of 2D materials is still barely explored. Herein, the covalentf unctionalization with silanes of am agnetic NiFe-LDH is reported. The synthetic route consists of at opochemical approach followed by anion exchange reaction with surfactant molecules prior to covalent functionalization with the (3-aminopropyl)triethoxysilane (APTES) molecules. The functionalized NiFe-APTES was fully characterized by X-ray diffraction, infrared spectroscopy, electron microscopy,t hermogravimetric analysis coupled with mass spectrometry and 29 Si solid-state nuclear magnetic resonance, among others. The effect on the electronic properties of the functionalizedL DH was investigated by am agnetic study in combination with Mçssbauer spectroscopy. Moreover,t he reversibility of the silane-functionalizationa t basic pH was demonstrated, and the quality of the resulting LDH was proven by studying the electrochemical performance in the oxygen evolution reaction in basic media. Furthermore, the anion exchange capability for the NiFe-APTES was tested employing Cr VI ,r esulting in an increase of 200 %o ft he anion retention. This report allows for an ew degree of tunability of LDHs, openingt he door to the synthesis of new hybrid architectures and materials.[a] Dr.Figure 2. FESEM (A), TEM (B) and mapping images (bottom panel) of NiFe-APTES. The inset in (A) shows DLS and the inset in (B) showst he SAED pattern. Mapping imagesare obtained from the single particle in the bottom left image( scale bar of 100 nm).