Self-organizing mechanical instabilities provide a promising route to programmatically micro/nanopatterning two-dimensional (2D) materials, which relies on deterministic control of instability-induced self-assemblies. However, due to ultra-low flexural rigidities, various non-deterministic multi-mode coupling mechanical instabilities are extremely prone to be triggered in 2D materials, which make it difficult to controllably self-assemble 2D nanocrystals into designed mode. Here, we report a deterministic mode of self-assembly in atomically thin 2D materials via mode-decoupled instabilities, which is the key to control self-assembled morphologies. Moreover, we capitalize on intermediate-multifunctional layers (IMLs) to construct 2D-materials/IML/substrate trilayer systems, which can implement three-order trans-scale directed and dynamic self-assemblies of 2D materials. Benefited from the unique properties induced by deterministic self-assemblies, we reported a concept for the fabrication of deterministically self-assembled micro/nano-electronics of 2D materials, such as ultra-fast gesture and anisotropic tactile sensors. The deterministic self-assemblies can considerably advance the development of post-programmable micro/nanopatterning technology and self-assembled electronics of 2D materials.

自组织机械不稳定性为编程微/纳米图案化二维 (2D) 材料提供了一条有前途的途径，它依赖于对不稳定性引起的自组装的确定性控制。然而，由于超低的弯曲刚度，二维材料极易引发各种不确定的多模耦合机械不稳定性，这使得二维纳米晶体难以可控地自组装成设计模式。在这里，我们通过模式解耦不稳定性报告了原子级薄二维材料中的确定性自组装模式，这是控制自组装形态的关键。此外，我们利用中间多功能层 (IML) 构建二维材料/IML/基板三层系统，可以实现三阶反式-二维材料的尺度定向和动态自组装。受益于确定性自组装所带来的独特特性，我们报告了一种用于制造二维材料的确定性自组装微/纳米电子产品的概念，例如超快速手势和各向异性触觉传感器。确定性自组装可以显着推进后可编程微/纳米图案技术和二维材料的自组装电子学的发展。