UiO-66 is an extremely versatile metal organic framework (MOF) due to its remarkable water stability and high specific surface area. The incorporation of modified chemical and structural defects (missing linker and missing cluster defects) into the crystalline UiO-66 by the simultaneous use of an amino modified ligand and a thiol containing monocarboxylic acid modulator (thioglycolic acid, TGA) during synthesis resulted in developing a novel dual-functional MOF, designated as NH2-UiO-66-SH_C. This material was characterized using FTIR, XRD, FESEM, EDX, XPS, BET and Zetasizer to explore the morphological integrity and chemical composition. NH2-UiO-66-SH_C crystals demonstrated irregular nano-sized morphology (< 100 nm) and microporous nature with specific surface area of 519.6 m2/g. The material was subsequently tested to adsorb the highly toxic aqueous mercury (Hg) which is responsible for severe damages to human health. The maximum adsorptive capacity for aqueous inorganic mercury was 885 mg/g at 303 K. The optimum adsorbent dose and solution pH were 0.3 g/L and 5, respectively. The adsorption was endothermic and followed pseudo-second order kinetics. The developed nano-adsorbent illustrated enhanced sorption capacities which were far higher compared to its parent MOFs (UiO-66 as well as NH2-UiO-66) and other reported modified forms of UiO-MOFs. A regeneration method that was effective over 5 cycles (Hg removal efficiency > 90%) was also reported. Overall, this study reports the development of a newly modified nano-crystalline MOF, by manipulation of the synthetic chemistry (with defect modulation), which is a promising adsorbent for Hg (II) in aqueous phase.