In order to realize a molecular-based conductor exhibiting three-dimensional intermolecular interaction, twin donors (1 similar to 4) have been designed. Electrocrystallization of the twin donor 1 gave three types of crystals (alpha-, beta-, and beta’-types). The crystal of alpha-type is composed of a pseudo cyclophane-shaped donor with 2:1 stoichiometry (1(2) . X, X = PF6-, BF4-, I-3(-), ClO4-), exhibiting a semiconducting character (Ea = 5X10(-2) eV). The crystal of beta-type is obtained as another morphology of ClO4- salts. The structure of the donor is a cyclophane-shape with short intramolecular S ... S distances. Insulating character of the salts can be rationalized mainly by the remote intermolecular S ... S distances. On the other hand, 1 . Cl .(H2O)(x) salts (beta’-type) shows a metallic conductivity. The difference in crystal structures between beta and beta’-type salts may be explained by introduction of a polymeric hydrogen-bonded counter ion system.