Transition metal-based layered double hydroxidesLayered double hydroxides (TM-LDHs) have emerged as promising materials for selective sorption, energy conversion, and storage applications due to their unique structural and electronic properties. The two-dimensional layered structure of TM-LDHs provides flexibility in accommodating different interlayer anions and metal cations in the bulk layer. The ability to tune the composition and structure of TM-LDHs makes them highly versatile for sorptive and catalytic applications. TM-LDHs demonstrate a significant potential in adsorbing a wide range of contaminants, including gases, volatile organic compoundsVolatile organic compounds, heavy metals, dyes, and emerging contaminants from aqueous and gaseous phases. Compared to the traditional LDH, the incorporation of transition metal in the LDH enhances the surface areaSurface area, porosityPorosity, and active sites, resulting in improved adsorption capacityAdsorption capacity. Additionally, the conductive nature of TM-LDHs provides the option for electro-assisted sorption and regeneration of the used adsorbentsAdsorbent. Nonetheless, the major hurdle in the real-time application of TM-LDH is the slow adsorption kinetics and poor stability at variable pH conditions. To overcome these limitations, strategies like nanostructuring, surface modificationSurface modification, and hybridizationHybridization with other materials should be explored. To this end, the current section of the monograph critically explores the advancements, present applications, and prospects of TM-LDHs as adsorbentsAdsorbent. The fundamental principles governing adsorption and the role of TM-LDH in state-of-the-art separations will be discussed. The separation mechanisms and the underlying adsorption properties that make TM-LDH suitable for the removal of heavy metals, anions (fluoride, nitrate, and phosphate), organic micropollutants, gas (carbon dioxide and nitrogen oxides), and volatile organic compoundsVolatile organic compounds will be communicated. Finally, the practical challenges and the potential of TM-LDHs to replace some of the current separation methods in terms of sustainabilitySustainability will be highlighted.