Two 1-D selenidoindates {[M(phen)(3)]In2Se5 center dot H2O}(n) (M = Ni, Fe) were synthesized by a solvothermal method. The 1-D {[In2Se5](2-)}(n) anion is a new type of single 1-D structure constituted by an alternately fused four-membered In2Se2 ring and five-membered In2Se3 ring. The chalcogenoindates were separated as mechanical racemic mixtures of single enantiomer crystals, in which the R-helix of 1-D InSe anion is directed by the related clockwise (Delta) cations of [M(phen)(3)](2+) or the L-helix of I-D anion is directed by the related anticlockwise (Lambda) cation. The pi center dot center dot center dot pi, C center dot center dot center dot Se, and C-H center dot center dot center dot Se oriented interactions of metal complex cations with selenidoindate anions play an important role in the formation of the chiral crystals. The embedded [M(phen)(3)](2+) cations improve the optical absorption of the 1-D semiconductor materials.