interactions of the catalytic nanoparticles resulting in unsatisfactory performance. [2] In an attempt to overcome the above shortcomings, noble metals were doped through self-assembly and layer by layer configuration on layered sheets of 2D materials (graphene sheets, MoS 2 , reduced graphene oxide, dichalcogenides, etc.) having high charge density and surface to volume ratio. [3][4][5][6] Additionally, the synthesis of these materials is chemical intensive and needs high temperature making the catalyst preparation unfavorable in terms of economic and energy considerations. Thus, the research focus in catalysis is now shifted to tailoring the geometry, electronic configuration, and charge density of the active metal. [7] Several ternary heterojunction compounds, complex and sandwiched geometry-based materials were synthesized to bridge the above-mentioned research gaps. However, a potential catalyst has less structural hindrance and better performance. Therefore, research on single-atom catalysis has gained attention due to the reason that the activity and stability of the catalysts attain the maximum when the size and distribution of the active metal approach the limit of a single atom. Another way to augment the performance and overcome the above limitations is by discretizing the active sites inside the ligand cavities. [8][9][10][11][12] Such flexibility regulates the local atomic arrangement controlling the surface properties easily.Anionic clays, like, layered double hydroxides (LDHs)where M 2+ is a divalent metal ion, M 3+ is a trivalent metal ion, and A n− is an n-valent anion) having exchangeable interlayer anions are suitable candidates as support materials that can be tuned to host the active metal in the interlayer. [13] LDHs are categorized under layered materials having positive lattice charge with intercalated anions, like, CO 3 2− , SO 4 2− , F − , OH − , NO 3 − , Cl − with basal spacing 0.7-0.88 nm. Additional features, like, high surface to volume ratio and charge density make the system versatile for such catalysis applications. Due to the structural heterogeneity, their applications include degradation of pharmaceutical components, organics, methanol oxidation reaction, oxygen evolution reactions, etc. [14][15][16] To enhance the activity of theseThe activity of the noble metal-based heterogeneous catalysts is limited by weak metal-support interactions, aggregation, and low surface to volume (S/V) ratio. The activity can be augmented in many ways. Among them, the discretization of the active sites and redistribution of electron density around the metal atom is an important one. In this work, these two phenomena are studied concerning a model reaction, hydrogenation of p-nitrophenol (p-NP). Herein, 1,4,7,10,13-pentaoxacyclopentadecane ether is introduced in the basal space of layered double hydroxide (LDH) to encapsulate noble Pd0 atom inside the cavity of the crown molecule strategically. The modified LDH (Pda-ECC-L0.10@in situ CoAl LDH) augments the properties, like, high S/V ratio and nonag...