To meet the growing demand of environmental protection and resource saving, it is imperative to explore bio-based elastomers as next-generation dielectric elastomers (DEs). In this study, we used a bio-based gelatin/glycerin (GG) elastomer as the DE matrix because GG exhibits high dielectric constant (ɛ r ). Cellulose nanocrystals (CNCs), extracted from natural cellulose fibers, were used to improve the mechanical strength of GG elastomer. The results showed that CNCs with a large number of hydroxyl groups disrupted the hydrogen bonds between gelatin molecules and formed new stronger hydrogen bonds with gelatin molecules. A good interfacial adhesion between CNCs and GG was formed, and thus a good dispersion of CNCs in GG matrix was obtained, leading to the improved mechanical strength of GG. More interestingly, the ɛ r of GG elastomer was obviously increased by adding 5wt% of CNCs, ascribed to the increase in the polarizability of gelatin chains caused by the disruption of hydrogen bonds of gelatin. As a result, a 230% increase in the actuated strain at low electric field of GG was obtained by adding 5wt% of CNCs. Since CNCs, gelatin and glycerol are all bio-based, this study offers a new method to prepare high performance DE for its application in biological and medical fields.