Circularly polarized luminescent (CPL) materials are currently drawing ever-increasing interest. This contribution reports the first success in simply combining chiral helical substituted polyacetylenes (HSPAs) with achiral luminophores to fabricate CPL materials demonstrating a high dissymmetry factor (g(lum)) up to 10(-1), despite neither covalent nor noncovalent interactions occurring between the two components. Circularly polarized scattering and fluorescence-selective absorption mechanisms are proposed for the generation of CPL, and a "matching rule" is further established for selecting chiral polymers and achiral luminophores for the purpose. Taking advantage of the circularly polarized scattering effect, full-color tunable CPL materials are prepared from the combination of achiral fluorescent dyes and chiral HSPAs. Following the fluorescence-selective absorption mechanism, functional composite films with on off and switchable CPL performance are fabricated. Also, remarkably, the g(lum) value in the prepared materials can reach up to +0.323. The present study provides a simple, powerful, and universal strategy for constructing novel CPL materials.