Crystalline aggregates containing metal cation clusters "wrapped" by reduced hydrocarbon anions have been presented. Initially, a dimeric complex (2) possessing a bimetallic K2O2 core was synthesized from the reaction between an anthracene substituted boronic acid (2-(anthracen-9-yOphenyl)(hydroxy)(mesityl)borane (1-H) and KN(SiMe3)(2) in THF solution. The B-O bond length (1.281(4) A) in complex 2 is comparable to those observed in oxoboranes, indicating this may be a double bond, which is supported by its Wiberg bond order (1.9) predicted by density functional theory calculations. Subsequently, potassium aggregate complexes, diradical 3 and dihydro anion 4, were obtained through the reduction reactions of dimeric complex 2 and 1-H, respectively. They exhibit similar K3O2B2 aggregate structures, but differ significantly in the geometry of the anthracene units. Complex 3 features a triplet diradical character with planar anthracene units that carry the unpaired electrons, while the anthracene groups in complex 4 display a puckered structure due to the addition of hydrogen atoms.