A catalyst-free, environmentally benign, and simple one-pot multi-component protocol has been developed for the efficient synthesis of novel (benzo[d]imidazo[2,1-b]thiazol-3-yl)-2H-chromen-2-one derivatives in excellent yields using ethanol-PEG-600. This novel and green protocol have the advantages of shorter reaction times, high conversions, and follow the group-assisted-purification (GAP) chemistry process, which can avoid traditional purifications, chromatography and recrystallization. This is the first report for the synthesis of benzo[d]imidazo[2,1-b]thiazol-3-yl)-2H-chromen-2-one.