Poor interfacial compatibility between unmodified cellulose nanocrystals (CNCs) and rubber restricts the property enhancement of matrix materials. In this study, according to structural similarity, the silylated CNC (SCNC) with diameter of 5–30 nm were prepared and incorporated into commercial silicone rubber (SR) via two-roll mill-compounding and vulcanization processes. As expected, at the same loading levels, SCNC had stronger reinforcing effect on the SR matrix than CNC. Compared to neat SR, with only 0.3 wt% (0.3 phr) SCNC1 incorporated, the tensile strength, Young’s modulus, storage tensile modulus, and maximum decomposition temperature (Tmax) of the nanocomposite were improved by 72, 125, 66 %, and 110.8 °C, respectively. Meanwhile the nanocomposites showed an obvious decrease in water vapor permeability (67 %). These enhancements were attributed to good dispersion of SCNC within SR matrix, improved interfacial interaction, and high crosslinking density.