The effect of deep eutectic solvents (DES) in devulcanization of ground tire rubber (GTR) was explored for the first time in this work. Three different DESs, namely ChCl:Urea, ChCl:ZnCl2 and ZnCl2:Urea were prepared and their physicochemical properties were examined. GTR was mixed with various DESs which were further sonicated and heated at various time intervals. The treated GTR was analyzed by energy dispersive X-ray (EDX), Fourier transform infrared spectroscopy (FTIR), field emission scanning electron microscope (FESEM) and thermogravimetric analysis (TGA). Additionally, the extent of devulcanization was assessed using soluble fraction, cross-link density and related by Horikx theory. The relation between DESs’ viscosities towards devulcanization efficiency was also evaluated.