<b>Nanolaminates composed of alternating layers of ZnO and Alb>2b>Ob>3b>b> are grown by conformal atomic-layer deposition. Their structural and nonlinear optical properties are correlated. Optimized nanolaminates exhibit an effective bulk second-order nonlinear optical susceptibility that is independent of the substrate and that is five times larger than that of potassium dihydrogen phosphate.