The fabrication of chiral molecules into macroscopic systems has many valuable applications, especially in the fields of optical displays, data encryption, information storage, and so on. Here, we design and prepare a serious of supramolecular glasses (SGs) based on Zn-L-Histidine complexes, via an evaporation-induced self-assembly (EISA) strategy. Metal-ligand interactions between the zinc(II) ion and chiral L-Histidine endow the SGs with interesting circularly polarized afterglow (CPA). Multicolored CPA emissions from blue to red with dissymmetry factor as high as 9.5 × 10−3 and excited-state lifetime up to 356.7 ms are achieved under ambient conditions. Therefore, this work not only communicates the bulk SGs with wide-tunable afterglow and large circular polarization, but also provides an EISA method for the macroscopic self-assembly of chiral metal–organic hybrids toward photonic applications.