Chiral 3D photonic crystals are an interesting subclass of 3D photonic crystals. For example, large complete 3D photonic bandgaps have been predicted for high-index-contrast silicon square-spiral structures; [1,2] corresponding experiments using glancing-incidence deposition, [3,4] interference lithography, [5] or direct laser writing [6,7] have been published. In addition to complete gaps or stop bands, theory [8] also predicts polarization stop bands, i.e., stop bands for just one of the two circular polarizations. Such polarization stop bands can give rise to strong circular dichroism, [4,9,10] which can potentially be used for constructing compact "thin-film" optical diodes. [11] In this report, we fabricate high-quality polymeric 3D spiral photonic crystals via direct laser writing. [12][13][14] The measured transmittance spectra of these low-index-contrast structures reveal spectral regions where the transmittance is below 5 % for one circular incident polarization and above 95 % for the other-for just eight lattice constants along the propagation direction. The experimental data are compared with scattering-matrix calculations [15,16] for the actual finite structures, leading to good agreement.For what conditions do we expect strong circular dichroism? For circular polarization of light, the tip of the electricfield vector simply follows a spiral. The pitch of this spiral is just the material wavelength k. Thus, intuitively, we expect a chiral resonance from spiral photonic crystals if the pitch of circularly polarized light matches the pitch of the dielectric spirals, i.e., the lattice constant a z . This condition, k/a z = 1, corresponds to the edge of the second Brillouin zone, i.e., to a wave number k z = 2p/k = 2p/a z . Recall that the edge of the first Brillouin zone is at k z = p/a z . Thus, one does not anticipate a strong chiral response around and below the fundamental stop band (or bandgap), but rather at higher frequencies. Theory [8] for high-index silicon-based structures confirms this intuitive reasoning. We have repeated similar calculations for low-index-contrast polymeric structures, revealing essentially the same trends. The parameters of the 3D spiral photonic crystals to be discussed below are the result of an optimization with respect to circular dichroism.The samples in our experiments are made by direct laser writing, which essentially allows for the fabrication of almost arbitrarily shaped 3D photoresist structures. [12][13][14] Details of our process based on the commercial thick-film resist SU-8 can be found in the Experimental section and in earlier work. [13] Our structures are mechanically supported by a 2D network of bars at, or close to, the top of the 3D crystal. As the spirals are not at all mechanically connected to their neighbors, very unstable low-quality structures would result without this grid. Furthermore, all the structures for optical experiments are surrounded by a thick massive wall (see Fig. 1a), which aims at reducing the effects of strain on the 2D grid cau...