Adding colloidal nanoparticles into liquid crystal media has become a promising pathway either to enhance or to introduce novel properties for improved device performance. Here we designed and synthesized new colloidal hybrid silica nanoparticles passivated with a mesogenic monolayer on the surface to facilitate their organo-solubility and compatibility in liquid crystal host. The resulting nanoparticles were identified by 1H NMR, TEM, TGA and UV-Vis techniques, and the hybrid nanoparticles were doped into a dual frequency cholesteric liquid crystal host to appraise both their compatibility with the host and the effect of the doping concentration on their electro-optical properties. Interestingly, the silica nanoparticle doped liquid crystalline nanocomposites were found to be able to dynamically self-organize into a helical configuration and exhibit multi-stability, i.e., homeotropic (transparent), focal conic (opaque) and planar states (partially transparent), depending on the frequency applied at sustained low voltage. Significantly, a higher contrast ratio between the transparent state and scattering state was accomplished in the nanoparticle-embedded liquid crystal systems.