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Physically cross-linked gels have unique advantages of repeated swelling and shrinking of network structures, where the stability of gels at the swelled phase, particularly under ionic conditions, is extremely critical. In this study, it has been shown that functionalized nanofillers and polar solvents can increase the network densities of physically cross-linked gels with higher dimensional stability by increasing the polar and electrostatic interactions. The characteristic nonbonded interactions of CNTs with ionic solvents have been utilized for the controlled swelling of toughened double-network gels as the function of pH and time. The swelling of the overall gel morphology is found to be important for the release of analytes; however, the functional cross-sectional sites in the nanohybrids hold the key for desorption kinetics. The selection of interactive functional moieties in the nanohybrids and analytes has led to the development of highly efficient and controlled release media. The electrostatic interaction of analytes with functionally and dimensionally stable gels with controlled porosity indicates a clear structure-property correlation, which could be exploited to design and fabricate efficient drug delivery vehicles and rapid surface decontaminants.