Two-dimensional (2D) materials and their engineered lattices offer exciting opportunities for next-generation electronic, optoelectronic, and electrochemical devices. Yet, studies of high-quality heterostructures have been largely constrained to microscopic flakes. Here, we present scalable, controllable top-down methods that transform a wide range of van der Waals (vdW) single crystals into twisted moiré superlattices with high yield, exceptional uniformity, and macroscopic dimensions from millimeters to centimeters. Access to such large-area structures has enabled new discoveries, including ultrafast thermal exchange at bilayer interfaces, rapid photoinduced tuning of moiré patterns, and markedly reduced Debye temperatures in deformed monolayers compared to their isolated counterparts. Furthermore, by patterning 1D features—such as nanoribbon arrays and nanowrinkles—on 2D monolayers, we uncover unique electronic and thermodynamic behaviors absent in pristine layers. These advances in large-scale 2D artificial structures pave the way toward mass production and practical deployment of twistronic devices.
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