Complex nematic fluids have the remarkable capability for selfassembling regular colloidal structures of various symmetries and dimensionality according to their micromolecular orientational order. Colloidal chains, clusters, and crystals were demonstrated recently, exhibiting soft-matter functionalities of robust binding, spontaneous chiral symmetry breaking, entanglement, shapedriven and topological driven assembly, and even memory imprinting. However, no quasicrystalline structures were found. Here, we show with numerical modeling that quasicrystalline colloidal lattices can be achieved in the form of original Penrose P1 tiling by using pentagonal colloidal platelets in layers of nematic liquid crystals. The tilings are energetically stabilized with binding energies up to 2500 k B T for micrometer-sized platelets and further allow for hierarchical substitution tiling, i.e., hierarchical pentagulation. Quasicrystalline structures are constructed bottom-up by assembling the boat, rhombus, and star maximum density clusters, thus avoiding other (nonquasicrystalline) stable or metastable configurations of platelets. Central to our design of the quasicrystalline tilings is the symmetry breaking imposed by the platelet shape and the surface anchoring conditions at the colloidal platelets, which are misaligning and asymmetric over two perpendicular mirror planes. Finally, the design of the quasicrystalline tilings as platelets in nematic liquid crystals is inherently capable of a continuous variety of length scales of the tiling, ranging over three orders of magnitude in the typical length (from ∼ 10 nm to ∼ 10 μm), which could allow for the design of quasicrystalline photonics at multiple frequency ranges.colloids | quasicrystals | Penrose tiling | hierarchy Q uasicrystals are aperiodic crystalline materials, distinguished by noncrystallographic rotational symmetry of fivefold, sevenfold, eightfold, and higher rotational symmetry axes (1-3). These symmetries are typically found in atomic lattices of distinct metallic alloys (1, 4). However, more recently, a unique class of soft-matter quasicrystals is emerging (5-8), where the basic building blocks are not single atoms but rather macromolecules (9, 10), copolymers (11), molecular liquid crystalline fields (12, 13), or colloidal particles (14, 15). Two-dimensional realizations of materials with quasicrystalline symmetries are quasicrystalline tilings (2,16,17). In tilings, the structures of polygons or platelets-tiles-cover an area in complex patterns, typically following geometric rules. Tilings with fivefold (18, 19), sevenfold (20), eightfold (21), ninefold (22), tenfold (23), twelvefold (24), and other (25) quasicrystalline symmetries were realized, demonstrating analogous ordering mechanisms as in quasicrystals (26,27). These ordering mechanisms and the formation dynamics were particularly explored in quasicrystalline colloidal monolayers stabilized by interfering laser beams (28,29).Nematic liquid crystals are fluids with molecular orientational order, called t...