LAUSR

The controlled preparation of single‐crystal Cu(111) is intensively investigated owing to the superior properties of Cu(111) and its advantages in synthesizing high‐quality 2D materials, especially graphene. However, the accessibility of large‐area single‐crystal Cu(111) is still hindered by time‐consuming, complicated, and high‐cost preparation methods. Here, the oxidization‐temperature‐triggered rapid preparation of large‐area single‐crystal Cu(111) in which an area up to 320 cm2 is prepared within 60 min, and where low‐temperature oxidization of polycrystalline Cu foil surface plays a vital role, is reported. A mechanism is proposed, by which the thin CuxO layer transforms to a Cu(111) seed layer on the surface of Cu to induce the formation of a large‐area Cu(111) foil, which is supported by both experimental data and molecular dynamics simulation results. In addition, a large‐size high‐quality graphene film is synthesized on the single‐crystal Cu(111) foil surface and the graphene/Cu(111) composites exhibit enhanced thermal conductivity and ductility compared to their polycrystalline counterpart. This work, therefore, not only provides a new avenue toward the monocrystallinity of Cu with specific planes but also contributes to improving the mass production of high‐quality 2D materials.