A new and highly efficient direct solvent, 1-allyl-3-methylimidazolium chloride (AMIMCI), has been used for the dissolution and regeneration of cellulose. The cellulose samples without any pretreatment were readily dissolved in AMIMCI. The regenerated cellulose materials prepared by coagulation in water exhibited a good mechanical property. Because of its thermostable and nonvolatile nature, AMIMCI was easily recycled. Therefore, a novel and nonpolluting process for the manufacture of regenerated cellulose materials using AMIMCI has been developed in this work.