A new series of morphologically stable, glassy chiral-nematic liquid crystals were synthesized following three distinct deterministic approaches. A glass transition temperature from 67 to 82 °C and a clearing temperature from 175 to 225 °C were accomplished. A helical pitch length from 188 to 210 nm emerged with enantiomeric 1-phenylethylamine as the precursors, giving rise to selective reflection in the UV region. With (+)-estrone as the chiral moiety, a selective reflection in the near-infrared was observed. The concepts of high-performance circular polarizers and optical notch filters and reflectors were illustrated with a mixture of enantiomeric glassy chiral nematics. Selective reflection wavelength can be readily tuned by varying chemical composition in terms of the ratio of enantiomers or that of chiral-nematic to nematic components.