AbstractThe synthesis of a macro-initiator from cellulose in mixtures of zinc-based ionic liquid and polar solvents including deep eutectic solvent, dimethylformamide, acetone, and tetrahydrofuran (THF) was studied. The results of FTIR and NMR spectroscopies indicated that the cellulose-based macro-initiator can only be obtained in an inert ether solvent, THF. When the amounts of cellulose and zinc-based ionic liquid were fixed at 0.5 g and 18 mL, respectively, the degree of substitution of the cellulose-based macro-initiator obtained was increased from 11.0% to 17.4% as the reaction temperature was increased from room temperature to 40 °C, as calculated from TGA thermograms. When the amount of cellulose was cut in half, a degree of substitution of 27.5% was achieved due to lower viscosity and better homogeneity of the reaction medium. A green, new, and relatively cheap approach has been shown to be suitable for synthesizing a cellulose-based macro-initiator.