Nd-substituted bismuth titanate (Bi3.5Nd0.5Ti3O12, BNdT) films were prepared on Pt electrodes using chemical solution deposition. Enhanced a-axis-oriented crystal growth occurred when the crystallization was performed on every spin-coated layer with sufficiently thin thickness (similar to 20 nm). The remnant polarization (2P(r) similar to 38 muC/cm(2)) of the film derived by such a layer-by-layer crystallization method was significantly higher than that of the film derived with the conventional process (2P(r)similar to10 muC/cm(2)). Examination of structural evolution has indicated that, owing to the geometrical effect, the growth of (1 1 7)-oriented crystals was restricted by the layer thickness, while the growth of a-axis-oriented crystals was not. As a result, BNdT films prepared by layer-by-layer crystallization are dominated by a-axis-oriented crystals and show high remnant polarization. (C) 2004 Elsevier B.V. All rights reserved.