Department of Chemistry, GITAM Institute of Science, GITAM University (Deemed to be), Visakhapatnam-530 045, Andhra Pradesh, India E-mail: duvvurisuryakala@gmail.com Manuscript received online 01 July 2020, accepted 31 August 2020 Structural analysis of extraordinary efficient CuO-CTAB (cetyl trimethyl ammonium bromide) and CuO-SDS (sodium dodecyl sulphate) nanoparticles and their adsorbing efficiency of significant dyes in aqueous media like Methylene blue, Rhodamine B and Congo red have been calculated using DFT calculations and compared with experimental studies. Structures of the active nano-cluster of (CuO)5, the most stable one derived by DFT methods is the most suitable for the adsorption of such dyes. Optimisations of the three aforementioned dyes have been performed and also the interactions on the CuO cluster have been performed using DFT calculations. A brief charge analysis for the dyes as well as the CuO nano-cluster has been performed, which also indicates the favorable adsorption and the sensor properties of such nano-clusters on different dyes. The quantum chemical descriptions are significant in explaining the adsorption of dyes on the copper(II) oxide at the respective active centers.