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We have continuously investigated crystal and electronic structures of a series of redox isomers of [Cr^III(SQ)_3-n(Cat)_n]^n�~ (SQ = o-semiquinonate and Cat = catecholate; n = 0-2) isolated as charge-transfer (CT) compounds. The ligand-based mixed-valence (LBMV) isomers have potentiality for creating novel molecular assembly constructed from supramolecular synthons such as SQ�E�E�ESQ magnetic type, SQ�E�E�ECat CT type, cation�E�E�ESQ, and cation�E�E�ECat interactions in terms of the oxidation state of the ligands. We will demonstrate unprecedented supramolecular assembly with several novelty, opening up possibilities for new materials and novel properties in the area of molecular assemblies