The self-organization of a third-order nonlinear optical metal complex, bis(dimethylglyoximato)platinum(II), Pt(dmg)(2), into one-dimensional chains is investigated. It is found that, upon vacuum evaporation on a KBr substrate, epitaxial crystallization of the metal complex takes place and plate-like islands are formed. Within the islands, the metal complex is organized into oriented chains of controllable length. The growth process and structure are discussed from optoelectronic and structural points of view.