CommuniCationeven larger than for bulk ZnO crystals. [4][5][6][7][8][9][10][11][12][13][14] These publications have also highlighted some of the important links between the structural properties of the thin films and their nonlinear optical susceptibility. In the work by Cao et al., thin films of ZnO were fabricated on sapphire substrates by pulsed laser ablation. [5] The second-order susceptibility was determined to be 13.40 pm V (2) 1. Furthermore, it was shown that the second-order susceptibility decreases with increasing crystalline quality and with increasing film thickness. This finding was attributed to a strong contribution of grain boundaries and interfaces to the second-order susceptibility. Another group highlighted the strong dependence of the structural and second-order nonlinear properties on the deposition conditions and the choice of the substrate. [4] Clearly, different deposition techniques lead to different growth behavior, hence different structural properties and thus different nonlinear optical properties. Atomic-layer deposition (ALD) is a fabrication technique that is particularly well-suited for the needs of optical integration. ALD is CMOS-compatible and allows for an inexpensive and conformal deposition on a large variety of substrates with a precision down to a monolayer. [15] Unfortunately, ZnO crystallites grown by ALD seem to have properties unfavorable for a strong second-order nonlinear response as there is not a single publication covering this topic. As we will show in this publication, the weak second-order response can be ascribed to the random orientation of the ZnO crystallites in pure ALD-grown ZnO thin films. In general, there are only few publications showing the realization of ALD-grown second-order nonlinear thin films and these are solely based on the idea of a strong interface-connected response. [16,17] In this Communication, we use the concept of nanolaminates to tune the second-order nonlinear properties as it has previously been demonstrated for the mechanical, linear optical, and also the third-order nonlinear optical properties of ALD-grown thin films. [18][19][20] Using this approach, we are able to control the ZnO crystallite growth and thus, for the first time, achieve a strong bulk second-order nonlinear susceptibility in ALD-grown thin films.The literature on ZnO thin films suggests that two key factors have to be controlled to maximize the second-order susceptibility in ALD-grown ZnO films. The first key factor is a well-defined ZnO crystallite orientation to avoid mutual cancellation of the contributions of neighboring misaligned crystallites. Without a preferential direction within a plane parallel to the substrate, the substrate normal is the only extraordinary direction. Indeed, ZnO films with a strong nonlinear