The iridescence of structural color and its polarization characteristics originate from the nanoscale organization of materials. A major challenge in materials science is generating the bright, lustrous hues seen in nature through nanoscale engineering, while simultaneously controlling interaction of the material with different light polarizations. In this work, a suitable chiral nematic liquid crystal elastomer ink is synthesized for direct ink writing, which self‐assembles into a chiral photonic structure. Tuning the writing direction and speed leads to the programmed formation of a slanted photonic axis, which exhibits atypical iridescence and polarization selectivity. After crosslinking, a freely programmable, chiroptical photonic polymer material is obtained. The strongly perspective‐dependent appearance of the material can function as specialized anticounterfeit markers, as optical elements in decorative iridescent coatings, or, as demonstrated here, in optically based signaling features. Inspired by natural examples of patterned iridescence, an ink based on a chiral nematic liquid crystal that can be processed with a direct ink writer 3D printer is shown. Tuning the writing direction and speed leads to the programmed formation of a slanted photonic axis that exhibits atypical iridescence and polarization selectivity.