The present study explores the utilization of naturally available organic acid-infused nano-adsorbents as effective ligands for the adsorption of Cr(VI) ions from aqueous samples. The nanomaterials were infused with natural organic acids using the solvent dispersion procedure. These infused organic acids play a crucial role in facilitating ligational interactions between metal ions and adsorbent particles. After the adsorption of Cr(VI) ions from 250 ppm aqueous dichromate solution the isolated adsorbent was leached with 2% nitric acid and assessed for Chromium content using Atomic absorption spectroscopy (AAS). Similarly, the regenerative efficacy of adsorbents was evaluated under thermal and electrolytic conditions using AAS. The ligational interactions of organic acids with metal ions and adsorbents was determined using Mass spectrometry. Among the natural acid ligands investigated, L-Glutamic acid demonstrated a notable increase in adsorption efficiency, reaching up to 33.5% when compared to non-infused control nano-adsorbents. This novel ligand-assisted adsorption strategy proves effective not only in adsorption but also in regenerating the adsorbents under thermal and electrolytic induction. L-Glutamic acid was found to be the most efficient facilitating agent for regenerative adsorbent design with Graphene-oxide which exhibited 20.1% Desorption rate which is approximately 5 times more than that of undoped Graphene-oxide, where as its efficiency further increased under electrolytic desorption with 21.3% of regeneration. The mass spectral analysis supports the metal-ligand interactions, particularly the prominent peak at m/z: 270.02, highlighting the robust Cr-L-Glutamic acid interactions over Graphene-oxide. The present study underscores the promising candidature of novel adsorbent systems by conglomerating Nano-adsorbents with natural organic acid ligands for prominent adsorption efficacy with substantial regeneration of adsorbent especially using Graphene-oxide-L-Glutamic acid system which offers promising avenues for the development of sustainable and effective remediation strategies for contaminated environments.