Photonic crystals (PCs) are an ideal framework to control optical nonlinear interactions. Since 1995, it has been shown that within a PC one may enhance, [1][2][3] phase match, [4,5] or hold a non-vanishing second-order interaction even if the material is centrosymmetric. [6] More recently, it has been pointed out that the structuring of the dielectric together with modulation of the second-order nonlinear susceptibility may lead to a backward parametric oscillation, [7] a nonlinear effect predicted many years ago that has not yet been observed. All such control over the nonlinear interaction is possible in 1D, 2D, or 3D PCs. Among them, 2D photonic structures are, perhaps, the most interesting, because such structures could, in principle, be easier to integrate into optoelectronic devices meant for light amplification, light generation at other frequencies, optical-data processing, or any kind of sensing. [8][9][10][11] The fabrication of 2D PCs using top-down procedures such as electron-beam lithography has been applied successfully in several kinds of semiconductors. [12][13][14] Unfortunately, patterning of inorganic crystals applying, for instance, focused-ionbeam bombardment and subsequent reactive-ion etching is limited to small depth/diameter ratios. [15] Developing procedures that would be more efficient in patterning inorganic crystals is very interesting for the fabrication of new light modulators that could take full advantage of the nonlinear optic and electro-optic coefficients of such materials. [16] On the other hand, neither the viability nor cost-effectiveness of integrating some very expensive nonlinear semiconductors in silicon-based devices have been clearly demonstrated. There are alternative routes to pattern inorganic nonlinear optical materials, such as KTiOPO 4 (KTP) or LiNbO 3 routes based on a periodical poling followed by a selective domain etching.[17]Although periodical poling has been applied with different degrees of success to obtain 1D arrays with a sub-micrometer period in some nonlinear materials, [18] it is still difficult to accurately control the size of small domains. Moreover, after poling one ends up with a stand-alone sample that would, certainly, be difficult to embed in any silicon-based device. We present here a completely novel combination of both topdown and bottom-up approaches to grow 2D PCs of KTP. These crystals are grown in ordered macroporous silicon templates. An additional benefit of such an approach is that, while being simple, the silicon matrix and the structured nonlinear material, which would eventually be used to modulate or generate light, forms an integral unit. To fabricate such a hybrid structure, an ordered silicon matrix of air holes and a KTP substrate were kept closely bound in a growth solution of KTP. We observed that KTP columns grew inside the air holes of the silicon matrix following the crystalline orientation of the substrate. Finally, the potential of the 2D array of KTP columns to control the nonlinear interaction was demonstrated by ...