Due to the interestingly tolerated physicochemical properties of deep eutectic solvents (DESs), they are currently in the process of becoming widely used in many fields of science. Herein, we present a novel Hg2+ adsorbent that is based on carbon nanotubes (CNTs) functionalized by DESs. A DES formed from tetra-n-butyl ammonium bromide (TBAB) and glycerol (Gly) was used as a functionalization agent for CNTs. This novel adsorbent was characterized using Raman spectroscopy, Fourier transform infrared (FTIR) spectroscopy, XRD, FESEM, EDX, BET surface area, and Zeta potential. Later, Hg2+ adsorption conditions were optimized using response surface methodology (RSM). A pseudo-second order model accurately described the adsorption of Hg2+. The Langmuir and Freundlich isotherm models described the absorption of Hg2+ on the novel adsorbent with acceptable accuracy. The maximum adsorption capacity was found to be 177.76 mg/g.