generation (SHG) or large linear electrooptic coefficients. [5][6][7][8] The entries of the second-order nonlinear optical susceptibility tensor have become comparable to and even larger than those of established crystalline materials such as KDP (monopotassium phosphate). [9] In sharp contrast to such crystals, laminate metamaterials can be deposited conformally onto any kind of amorphous surface by atomiclayer deposition (ALD), enabling the integration into various systems. [10] In this Communication, we investigate the possibility of enhancing the secondorder frequency-conversion efficiency by bringing together the ideas of 3D dielectric photonic crystals and dielectric laminate metamaterials. Due to their hybrid nature, we refer to these structures as "3D laminate metacrystals" (see Figure 1a).An obvious advantage of this hybrid approach is based on the fact that ALD is a conformal process. Therefore, the overall amount of material grown after some time in a structure with N inner surfaces is N-times larger than that grown on a single planar surface during the same time. This is a relevant aspect, because ALD does not allow for growing films with thicknesses of tens of micrometers on planar surfaces within reasonable time. Originally, we anticipated two further advantages of this hybrid approach: nonlinear optical phase matching by the dispersion relation of photonic crystals and enhanced nonlinearities by small group velocities ("slow light") near the extrema of photonic bands. [11][12][13][14][15][16][17] However, these aspects turned out to be of minor importance for the understanding of the resonances observed in this report.The samples have been fabricated as follows. We start by manufacturing 3D woodpile polymer templates on glass substrate by using a home-built setup for 3D direct laser writing. [18,19] Ordinarily, one uses photoinitiator molecules in a monomer to support efficient two-photon absorption required in the direct laser writing process. [20] However, the photoinitiator molecules lead to two-photon-induced fluorescence in the final structures. This fluorescence can largely obscure the SHG measurements. Therefore, we use an acrylate resist without any additional photoinitiator and directly excite optical transitions in the monomer by tightly focused femtosecond laser pulses centered at 405 nm wavelength (see the Experimental Section for further details). Despite the absence of a photoinitiator, we will still report on remaining polymer autofluorescence below.We have varied the rod spacing, a, the axial lattice constant, c, and the rod cross section of the resulting woodpile photonic crystals. A ratio of = / 2 c a leads to a face-centered cubic diamond-like lattice, a ratio of c/a = 1 to a body-centered cubic 3D dielectric woodpile photonic crystals, which are conformally coated with locally noninversion-symmetric dielectric laminate metamaterials, are discussed. These "3D laminate metacrystals" are fabricated by 3D direct laser writing of an acrylate without photoinitiator to reduce two-photo...