Here we report a novel chiral smectic through self-assembling two-dimensional graphene oxide nanosheets and one-dimensional cellulose nanorods. As shown by a phase diagram, the formation of the chiral smectic strictly depends on the ratio of nanosheets to nanorods as well as the concentration of the composite colloid. It would open up a new way for the development of mesoscopic materials with tunable physical properties, such as optical metamaterials with application in optical modulation and mechanochromic sensors.