in terms of the number of MOFs synthesized over the past two decades for a variety of applications, MOFs with high iodine uptake capacity remain conspicuously sparse. [7] 129 I is one of the most hazardous radioisotopes in nuclear waste with a long radioactive half-life of 1.57 × 10 7 years. Several adsorbents that include chalcogenides, aerogels, functionalized clays, silver-based porous zeolitic materials, etc. with loading amounts ranging from 8 to 175 wt% have been reported. [8][9][10] However, their application is precluded by one or the other of the disadvantages such as high cost, limited adsorption ability, and serious environmental effects. The materials with better high-iodine trapping ability are a need of the hour. In general, adsorption capacity for iodine by porous materials is related not only to the pore size but also to other important factors such as effective availability of sorption sites, I 2 -framework interactions, composition/ratio of I 2 and polyiodide anions. One of the important ways to develop materials with high iodine capture is to introduce π-conjugated organic ligands, pyridines with readily available electron pairs and electron-rich functional groups such as OH, NH 2 , NR 2 , and COOH, which permit either formation of stable charge-transfer complexes or stronger halogen bonds with iodine; electron-rich moieties are expected to enhance charge-transfer interactions and hence the efficiency of adsorption of iodine. [11][12][13][14][15][16][17] The properties of any porous material are determined by constituent building blocks, pore attributes, and characteristics of the exposed surface area. As compared to 3D MOFs, the analogous lower dimensional 2D metal-organic nanosheets (MONs) have garnered much attention in the last few years [18][19][20][21][22][23][24][25] since the discovery of graphene and its burgeoning applications in diverse domains. [26][27][28][29][30][31][32][33][34][35][36][37][38][39][40][41] An important feature of MONs is the high surface area, which allows better interaction with guest molecules. Due to the ultrathin nature of the sheets, [42] large surface area, high ratio of surface area-to-volume, [43] and readily accessible active sites, MONs have been tremendously explored for gas separations, [30][31][32][33][34][35] energy storage and conversion, [38] catalysis, [28] sensing, [34,39] etc. The synthesis of 2D MONs is a challenge, as the growth of the crystals is a limiting factor. Several synthetic strategies have now been developed for MONs, which include bottom-up and top-down approaches. [19][20][21][22][23] The former is a straightforward direct synthesis of nanosheets from An electron-rich π-conjugated organic linker H 4 BPDP (BPDP = biphenyl dipyrrole tetracarboxylic acid) is designed and subjected to metal-assisted self-assembly to afford a layered metal-organic framework (MOF), i.e., Cd-BPDP. Single crystal X-ray structure determination and analysis show that two corrugated layers of the MOF are intertwined to yield thick strands of porous 2D metal-o...