<p>Circularly polarized luminescence (CPL) materials have attracted great attention because of their rich optical information and excellent sensitivity. However, the strategy to prepare CPL materials with a high dissymmetry factor (<i>g</i>) is still limited. Herein, we demonstrate a facile route to scale up the fabrication of circularly polarized organic room-temperature phosphorescent (CP-RTP) materials with a high <i>g</i> value, outstanding flexibility and complete biodegradability, via the reconstruction and enhancement of hydrogen-bonding interactions of cellulose. The absorption dissymmetry factor (g<sub><i>abs</i></sub>) and luminescence dissymmetry factor (g<sub><i>lum</i></sub>) of the CP-RTP materials are as high as 0.48 and 0.16, respectively, which are one or two orders of magnitude larger than previous records. These cellulose-based CP-RTP materials have full-color emission, and can be processed into different format. In particular, the CP-RTP materials exhibit chiral recognition performance in an instrument-free visual mode. They give a change of RTP performance once meeting different enantiomers, including lysine, histidine, cysteine, 2-chloromandelic acid, and 1-(2-naphthyl) ethanol. The novel strategy and new CP-RTP materials could promote the enrichment and practical applications of CPL materials.</p>