Moiré patterns arise either from twisting the same materials at a specific angle or from a lattice mismatch between different materials (Figure ). In this study, we focused on Moiré patterns formed by the former method. Following the exfoliation of the MOF nanosheets using sonication, we observed Moiré patterns at various twist angles for Zr-NDC, Zr-BPDC, and Zr-AZDC (Figures and). We determined the twist angles of the twisted bilayer MOFs using TEM measurements, with the fast Fourier transform (FFT) patterns facilitating the identification of these angles. The TEM images were consistent with the simulated images. As the twist angle increased, the Moiré pattern decreased. In addition, the Moiré patterns gradually enlarged as the ligand length of the MOFs increased from NDC to BPDC and AZDC. Due to the higher electron density of Zr clusters compared to the organic components, FFT spots originated from the arrangement of Zr clusters within the triangular lattice. We also observed satellite peaks in the FFT patterns of the Moiré TEM images (Figure ). This phenomenon has been noted in another Moiré material, twisted bilayer graphene, and is attributed to diffuse scattering. Furthermore, we investigated the common angles observed in the Zr-BPDC MOF. Approximately one hundred TEM images were collected from the twisted bilayer Zr-BPDC, revealing no distinct preference for twist angles. A broad distribution of twist angles was observed, with a relatively higher proportion of bilayers exhibiting angles around 10 degrees (Figure ). Figure presents representative TEM images showing the various Moiré patterns observed in the twisted bilayer Zr-BPDC (see also Figures ).