Quasicrystalline superlattices (QC-SLs) generated from single-component colloidal building blocks have been predicted by computer simulations but are challenging to reproduce experimentally. We discovered that 10-fold QC-SLs could self-organize from truncated tetrahedral quantum dots with anisotropic patchiness. Transmission electron microscopy and tomography measurements allow structural reconstruction of the QC-SL from the nanoscale packing to the atomic-scale orientation alignments. The unique QC order leads to a tiling concept, the “flexible polygon tiling rule,” that replicates the experimental observations. The keys for the single-component QC-SL formation were identified to be the anisotropic shape and patchiness of the building blocks and the assembly microscopic environment. Our discovery may spur the creation of various superstructures using anisotropic objects through an enthalpy-driven route.