Quasicrystals are long-range ordered and yet non-periodic. This interplay results in a wealth of intriguing physical phenomena, such as the inheritance of topological properties from higher dimensions, self-similarity, and the presence of non-trivial structure on all scales. The concept of aperiodic order has been extensively studied in mathematics and geometry, exemplified by the celebrated Penrose tiling. However, the understanding of physical quasicrystals (the vast majority of them are intermetallic compounds) is still incomplete owing to their complexity, regarding both growth processes and stability. Ultracold atoms in optical lattices offer an ideal, yet untested environment for investigating quasicrystals. Optical lattices, i.e. standing waves of light, allow the defect-free formation of a large variety of potential landscapes, including quasiperiodic geometries. In recent years, optical lattices have become one of the most successful tools in the large-scale quantum simulation of condensed-matter problems. This study presents the first experimental realisation of a two-dimensional quasicrystalline potential for ultracold atoms, based on an eightfold symmetric optical lattice. It is aimed at bringing together the fields of ultracold atoms and quasicrystals – and the more general concept of aperiodic order. The first part of this thesis introduces the theoretical aspects of aperiodic order and quasicrystalline structure. The second part comprises a detailed account of the newly designed apparatus that has been used to produce quantum-degenerate gases in quasicrystalline lattices. The third and final part summarises the matter-wave diffraction experiments that have been performed in various lattice geometries. These include one- and two-dimensional simple cubic lattices, one-dimensional quasiperiodic lattices, as well as two-dimensional quasicrystalline lattices. The striking self-similarity of this quasicrystalline structure has been directly observed, in close analogy to Shechtman’s very first discovery of quasicrystals using electron diffraction. In addition, an in-depth study of the diffraction dynamics reveals the fundamental differences between periodic and quasicrystalline lattices, in excellent agreement with ab initio theory. The diffraction dynamics on short timescales constitutes a continuous-time quantum walk on a homogeneous four-dimensional tight-binding lattice. On the one hand, these measurements establish a novel experimental platform for investigating quasicrystals proper. On the other hand, ultracold atoms in quasicrystalline optical lattices are worth studying in their own right: Possible avenues include the observation many-body localisation and Bose glasses, as well as the creation of topologically non-trivial systems in higher dimensions.