To further investigate the energy dependence on twist angles, a superstructure of Zr-BPDC MOF was constructed. This superstructure is composed of bilayers, with each layer consisting of 37 Zr clusters (Supplementary Information Section 3). Given the exceedingly large number of atoms, conducting density functional theory calculations was infeasible. Therefore, we employed the molecular dynamics method to calculate the energy at specific twist angles. For the simulations, we generated a bilayer MOF by rotating one layer around the central metal cluster at a specific angle (Figure ). Figure shows the total energy of the twisted bilayer Zr-BPDC as a function of the twist angle. Remarkably, the observed trends in the TEM images align with the average energy graphs (Figures and). The energy profile exhibits a global minimum value in the range of 10 to 15 degrees.