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A bifunctional MOF for selective CO2 capture and efficient aqueous‐phase sensing of 2,4,6‐trinitrophenol (TNP) has been rationally designed and synthesized. Owing to the presence of basic (−NH2) functionalized pore surface, the MOF exhibits selective adsorption of CO2 with a high value of heat of adsorption (Qst = 46.5 kJ mol−1) which is about 10 kJ mol−1 higher than that of the analogues MOF without −NH2 functionality. Further, the MOF shows highly selective, aqueous‐phase sensing of TNP over other competing NACs. The observed selectivity of MOF for CO2 capture and sensing of TNP has been correlated to the stronger interaction of the guest molecules with the basic −NH2 groups in the 1D channels, unveiled from the DFT calculations. For more information see the Full Paper by C. M. Nagaraja et al. on page 16204 ff.

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