The production of large-area twisted bilayer graphene (TBG) with controllable angles is a prerequisite for proceeding with its massive applications. However, most of the prevailing strategies to fabricate twisted bilayers face great challenges, where the transfer methods are easily stuck by interfacial contamination, and direct growth methods lack the flexibility in twist-angle design. Here we develop an effective strategy to grow centimetre-scale TBG with arbitrary twist angles (accuracy, <1.0°). The success in accurate angle control is realized by an angle replication from two prerotated single-crystal Cu(111) foils to form a Cu/TBG/Cu sandwich structure, from which the TBG can be isolated by a custom-developed equipotential surface etching process. The accuracy and consistency of the twist angles are unambiguously illustrated by comprehensive characterization techniques, namely, optical spectroscopy, electron microscopy, photoemission spectroscopy and photocurrent spectroscopy. Our work opens an accessible avenue for the designed growth of large-scale two-dimensional twisted bilayers and thus lays the material foundation for the future applications of twistronics at the integration level.

制备具有可控角度的大面积扭曲双层石墨烯（TBG）是其大规模应用的先决条件。然而，大多数制造扭曲双层的主流策略都面临着巨大的挑战，其中转移方法很容易被界面污染卡住，而直接生长方法在扭曲角设计方面缺乏灵活性。在这里，我们开发了一种有效的策略来生长具有任意扭转角（准确度，<1.0°）的厘米级 TBG。精确角度控制的成功是通过从两个预旋转的单晶 Cu(111) 箔进行角度复制以形成 Cu/TBG/Cu 夹层结构来实现的，TBG 可以通过定制开发的等电位表面蚀刻工艺从中分离出来. 通过综合表征技术，即光学光谱、电子显微镜、光电子能谱和光电流光谱，可以清楚地说明扭转角的准确性和一致性。我们的工作为大规模二维扭曲双层的设计增长开辟了一条可行的途径，从而为扭曲电子学在集成层面的未来应用奠定了物质基础。