Cathodic electrodeposition in an aqueous mixed solution of zinc nitrate and water-soluble tetrasulfonated metallophthalocyanines (TSPcMs), in which M = Zn(II) (TSPcZn), Al(III)[OH] (TSPcAl), or Si(IV)[OH]2 (TSPcSi), resulted in a self-assembled growth of zinc oxide (ZnO) thin films whose surface is modified by TSPcMs. It has been found that the adsorption of TSPcM onto the growing surface of ZnO strongly affects the crystal growth and the orientation of the ZnO crystallites. The effect was most prominently seen with TSPcSi, creating a film looking like stacking disks aligned perpendicular to the substrate. Crystallographic studies by X-ray diffraction and TEM observation coupled with the selected area electron beam diffraction have revealed that thin platelike crystals, whose planes and edges correspond to the (002) and (100) crystal faces, respectively, are aligned in the same orientation around the c-axis within the stacks. The evolution of this unique structure is interpreted as arising from the prefer...