Through mathematical derivation, we established that twisted bilayer MOFs with a twist angle of 30 degrees exhibit an aperiodic structure. Notably, this aperiodic pattern, characterized by a lack of translational symmetry, possesses twelve-fold rotational symmetry. The agreement between calculated and observed FFT patterns and TEM images strongly indicated the dodecagonal quasiperiodic structures of Zr-NDC, Zr-BPDC, and Zr-AZDC (Figures S7-S9 and S19). To map the quasiperiodic pattern of the MOFs without gaps or overlaps, we employed a Stampfli-tiling, composed of triangles, squares, and rhombuses. The Stampfli tile exhibits a fractal structure with self-similarity, where the same pattern repeats on larger scales with an irrational scaling factor of √ 2 + √3 (Figure ). When comparing the model structures of the tiles, representing the 3 rd inflation in the fractal structure, with the corresponding regions in the TEM image of Zr-BPDC, significant alignment was observed (Figure ). Furthermore, the TEM images in Figure clearly showed triangle, square, and rhombus tiles with increasing edge lengths of 6.13, 6.85, and 7.57 nm within the isoreticular series of MOFs. This observation demonstrates successful control over the length scale of the dodecagonal quasiperiodic pattern. The length of tiles in 1 st inflation (l1) is 𝑎 𝑀𝑂𝐹 • cos 15°, where 𝑎 𝑀𝑂𝐹 is 1.7, 1.9, 2.1 nm for Zr-NDC, Zr-BPDC, and Zr-AZDC.