The present manuscript reports the synthesis of multistimulus-responsive smart supramolecular hydrogels derived by in situ coating of silver nanoparticles (Ag NPs) on colloidal cytidine-5′-monophosphate-capped β-FeOOH nanohybrids (β-FeOOH@5′-CMP) under physiological conditions forming a polycrystalline building block (Ag-coated β-FeOOH@5′-CMP). The presence of Ag in the binary nanohybrids induces the puckering of ribose sugar, bringing a change in its conformation from C2′-endo to C3′-endo, which enhanced the supramolecular interactions among different moieties of other building blocks to construct a porous network of hydrogels in the self-assembly via the formation of a micellar structure. Such a supramolecular network in hydrogel is also evidenced by the reversible sol⇌gel transformation under multistimulus-responsiveness in a narrow range of pH, temperature, and sonication, as well as by the manifestation of rapid self-healing and injectability features. As-synthesized hydrogels exhibiting shear-thinning behavior under higher strain and converting back into the sol under low strain, suggests their potential for localized drug delivery. The presence of Ag NPs in the hydrogel enhanced its viscoelastic properties, % swelling (580) and loading capabilities (590 mg g-1) for methylene blue (MB), and its controlled release over days (∼2-30) as a function of pH. It displayed excellent surface-enhanced Raman spectroscopy activity allowing to detect MB-like drug molecules at ≤10-12 M. Thus, the as-synthesized hydrogels represent a unique superparamagnetic nanosystem consisting of all greener components (5′-CMP/β-FeOOH/Ag) with superior viscoelastic, sensing, and antimicrobial properties, displaying multistimulus-responsiveness (pH/temperature/sonication), thereby suggesting their vast potential for biomedical and environmental applications. © 2020 American Chemical Society.