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The new nanoporous framework [Gd 4 (di-nitro-BPDC) 4 (NO 2 ) 3 (OH)(H 2 O) 5 ]•(solvent) (I; di-nitro-BPDC 2− = 2,2′-dinitrobiphenyl-4,4′-dicarboxylate) has been designed and synthesized through a simple one-pot reaction. In addition to its exceptional thermal and water stabilities, I exhibited multifunctional properties. A sudden CO 2 uptake to a maximum of 4.51 mmol g −1 (195 K and 1 bar) with notable selectivity over O 2 and N 2 (CO 2 /O 2 = 39 at 195 K and 0.10 bar, CO 2 /N 2 = 46 at 195 K and 0.10 bar) and an isosteric adsorption enthalpy of 20.7(4) kJ mol −1 have been revealed. Depending on the temperature and humidity, I also showed distinguished superprotonic conductivities with a maximum value and activation energy of 6.17 × 10 −2 S cm −1 (55 °C, 99 RH%, and 1 V AC voltage) and 0.43 eV, respectively. With respect to the linear dependence of conductivities on both temperature (25−55 °C at 99 RH%) and humidity (55−99 RH% at 25 °C), the potential of I in temperature and humidity sensing was evaluated, disclosing an excellent sensing resolution and exceptional accuracy, precision, and repeatability for the measurements.

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