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We report an interesting interaction between oxidized multiwalled carbon nanotubes (oxi-MWCNTs), tetra n-heptylammonium bromide (ionic liquid) and total chromium ((Cr(VI)/Cr(III)) in this study. The interaction between the IL and oxidized MWCNTs primarily involves electrostatic affinity between the quaternary ammonium cation, and surface carboxyl and hydroxyl groups in oxi-MWCNTs. The IL-oxi-MWCNT adsorbent acts as a host in welcoming the incoming guest hydrochromate anions and several interesting interactions such as cation–π interactions, electrostatic interactions as well as anion–π interactions could be conceptualized in this process. The abundant oxygen-containing functional groups on the surfaces of oxi-MWCNTs play an important role in Cr(VI)/Cr(III) sorption. Characterization of the adsorbent was performed using various characterization techniques such as cross polarization magic angle …