Polymer-dispersed liquid crystal (PDLC) and polymer-stabilized liquid crystal (PSLC) are two typical liquid crystal (LC)/polymer composites. PDLCs are usually prepared by dispersing LC droplets in a polymer matrix, while PSLC is a system in which the alignment of LC molecules is stabilized by interactions between the polymer network and the LC molecules. In this study, a new material system is promoted to construct a coexistence system of PDLC and PSLC, namely PD&SChLC. In this new material system, a liquid-crystalline vinyl-ether monomer (LVM) was introduced to a mixture containing cholesteric liquid crystal (ChLC) and isotropic acrylate monomer (IAM). Based on the different reaction rates between LVM and IAM, the PD&SChLC architecture was built using a stepwise UV-initiated polymerization. During the preparation of the PDS&ChLC films, first, the mixture was irradiated with UV light for a short period of time to induce the free radical polymerization of IAMs, forming a phase-separated microstructure, PDLC. Subsequently, an electric filed was applied to the sample for long enough to induce the cationic polymerization of LVMs, forming the homeotropically-aligned polymer fibers within the ChLC domains, which are similar to those in a PSLC. Based on this stepwise UV-initiated radical/cationic polymerization, a PD&SChLC film with the advantages of a relatively low driving voltage, a fast response time, and a large-area processability is successful prepared. The film can be widely used in flexible displays, smart windows, and other optical devices.