Zinc metal was vacuum deposited at room temperature onto cadmium stearate Langmuir-Blodgett (LB) films with surfaces of either hydrophilic head groups or hydrophobic tail groups. Different growth modes on different surfaces of the LB films were observed with an atomic force microscope (AFM). Fine Zn particles deposited onto the hydrophobic surface were uniform and similar in shape irrespective of the deposition rate. However, on the hydrophilic surface, triangular and/or quasi-hexagonal Zn crystals were observed when the deposition rate was very low. Chemical interaction between organic functional groups and deposited metal seems critical for the manner of growth. The possibility of control of the architecture over inorganic crystallization using two-dimensionally oriented organic surfaces is proposed.