We report the fabrication and characterization of a pHresponsive hydrogel with improved mechanical and dielectric properties from cellulose nanocrystals. X-ray diffraction and SEM observations were used to analyze the sample morphology. The resulting pH detector exhibits a pronounced change in their swelling index in response to variation in pH. It was used singly and in combination with other nanomaterials to optimize smart material designs. The applications of the developed material are anticipated in chemical, environmental and biological systems.