Circularly polarized luminescent carbon dot nanomaterials of self-organized helical superstructures based on cellulose nanocrystals enable strong, right-handed, and multicolor tunable circularly polarized luminescence with extraordinary dissymmetry factors up to −0.74. The effects of emission intensity and carbon dots loading on the strength of the right-handed circularly polarized luminescence are experimentally observed and theoretically explained. Potentials of the carbon dots–cellulose nanomaterials for circularly polarized light detection are demonstrated.