In this work, we validate that cellulose nanocrystals (CNCs), surface-functionalized with pro-mesogenic azobenzene pendants, can act as photoswitchable chiral solutes in a nematic liquid crystal (N-LC). Upon UV illumination, the helical pitch and thus the helical twisting power (beta(w)) can be altered based on the trans-cis photoisomerization of the azobenzene pendants. This approach shows that CNCs-biorenewable chiral additives with a commensurate, rod-like shape to N-LC molecules-can be adapted just like common small molecule organic chiral solutes in LC phases based on simple surface modifications.