Recently, chirality was successfully introduced to rare earth complexes, which have long afterglow phosphorescence, by ball-milling with l/d-cysteine, leading to CPP with a dissymmetry factor (g lum ) up to 10 −2 . [16] CPP from multiple metal centers has also been achieved by the preparation of a homochiral metal-organic framework. [17] Despite these fantastic examples, the candidates for creating CPP are still limited. New candidates with a long lifetime and intrinsic phosphorescence are urgently needed to widen the family of CPP materials and broaden the scope of their applications.Metal nanoclusters (NCs) are intermediates between single-metal complexes and metal nanoparticles. [18,19] Metal NCs, especially those formed by the complexation of metal ions with organic ligands, could have atomic precision proved by single-crystal X-ray diffraction analysis. Their photoluminescence is normally weak in dilute dispersions or amorphous state, which is disadvantageous for the construction of CPP materials. However, this drawback could be overcome by lowering the temperature or forcing them to form highly ordered supramolecular structures. [20] In the latter case, in most cases, the emission is characterized by a relatively long lifetime of microseconds that could be assigned to phosphorescence in nature. For the chirality which is another necessity to induce CPP, chiral organic ligands were routinely adopted during the preparation of the metal NCs. [21][22][23][24][25][26][27][28][29][30][31][32][33][34][35] Based on these efforts, a few metal NCs that exhibit CPP in solid states have been successfully created, including gold, [27][28][29] silver, [30,31] and copper [32][33][34][35] NCs.In terms of the chirality of a given system, the building blocks are unnecessarily chiral, which has been confirmed by chiral supramolecular self-assemblies formed by achiral organic molecules, such as those with C 3 -symmetry. [36][37][38] However, this rule has not been demonstrated for metal NCs until very recently. [39] The breakthrough came from the assembly of watersoluble silver NCs ((NH 4 ) 9 [Ag 9 (mba) 9 ], H 2 mba = 2-mercaptobenzoic acid, abbreviated to Ag 9 -NCs hereafter), which were facilely obtained by coordination of Ag(I) with 2-mercaptobenzoic acid (H 2 mba) in water in the presence of ammonia-water (Figure 1a). Single-crystal X-ray diffraction analysis showed each cluster has a core of nine Ag(I) ions that resembles a triangular prism comprising three Ag 3 trigons. The cluster has a C 3 axis that passes Recently, advanced optical materials with circularly polarized phosphorescence (CPP) have attracted much attention. However, such materials are limited due to the difficulty of preparation and the scarcity of precursors. Herein, CPP materials are constructed for the first time using water-soluble, pseudo-chiral silver nanoclusters with atomic precision ((NH 4 ) 9 [Ag 9 (mba) 9 ], H 2 mba = 2-mercaptobenzoic acid, abbreviated to Ag 9 -NCs hereafter). Induced by the complexation of l-or d-tartaric acid (TrA) through h...