SynopsisCongo red bound to regenerated cellulose in highly swollen gel films formed by slow precipitation from LiCl/N,N-dimethylacetamide solution exhibits induced optical activity. The induced CD band of the dye vanishes when these films are dried under uniaxial stress, indicating that the effect is structural in origin and not simply due to association of dye with chiral centers on the cellulose chain. Cellulose was also regenerated from cellulose acetate films, cast both from isotropic and cholesteric solution, by deacetylation in aqueous ammonia. Congo red bound to cellulose regenerated from cholesteric cellulose acetate exhibits an induced CD band similar to that obtained for films precipitated from LiCl/DMAC solution. The CD spectrum of Congo red in cellulose films regenerated from isotropic cellulose acetate is featureless. These observations indicate that cellulose adopts cholesteric order on slow precipitation from solution.