Cholesteric liquid crystal (CLC) materials used in electro-optical (EO) devices are characterized by high operating voltage and slow response speed, which hinders their further development in display applications. Dual-frequency CLCs (DFCLCs) can solve the problem of slow bistable transition, but the operating voltage is still high, especially in colorreflective DFCLC cells. Here we report a simple approach to lowering the switching voltage as well as to shortening the response time. This technique adopts hybrid surface treatment to modulate the structural arrangement of CLC molecules. Both planar- and vertical-alignment layers are employed and coated on one and the other substrates separately to improve the electro-optical properties of DFCLCs. We show that the threshold voltage for switching can be decreased to as low as 5 V and the shortest response time is measured to be 0.8 ms, which renders CLC EO devices including displays more practical for commercial purpose.