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A simple and general method is presented herein for the in situ preparations of circularly polarized luminescence (CPL)‐active microcrystals with a large luminescence dissymmetry factor glum, high fluorescence quantum efficiency (ΦFL), wide emission color tenability, and well‐ordered morphology. The reactions of pyridine‐containing achiral molecules 1–7 with chiral camphor sulfonic acid ((±)‐CSA) gave crystalline microplates formed by hydrogen bonding interactions between the protonated pyridinium units and the sulfonic anions. The chiral information of CSA are effectively transferred to the microcrystals by hydrogen bonding to afford full‐color CPL from deep‐blue to red with glum in the order of 10−2 and ΦFL up to 80 %. Moreover, organic microcrystals with high‐performance white CPL (ΦFL=46 %; |glum|=0.025) are achieved via the light‐harvesting energy transfer between blue and yellow emitters. [ABSTRACT FROM AUTHOR]