Light may carry both orbital angular momentum (AM) and spin AM. The former is a consequence of its helical wavefront, and the latter is a result of its rotating transverse electric field. Intriguingly, the light–matter interaction with such fields shows that the orbital AM of light causes a physical “twist” in a range of materials, including metal, silicon, azopolymer, and even liquid-phase resin. This process may be aided by the light’s spin AM, resulting in the formation of various helical structures. The exchange between the AM of light and matter offers not only unique helical structures at the nanoscale but also entirely novel fundamental phenomena with regard to the light–matter interaction. This will lead to the future development of advanced photonics devices, including metamaterials for highly sensitive detectors as well as reactions for chiral chemical composites. Here, we focus on interactions between the AM of light and azopolymers, which exhibit some of the most diverse structures and phenomena observed. These studies result in helical surface relief structures in azopolymers and will leverage next-generation applications with light fields carrying optical AM.