effects, quantum interference, nuclear spins, and electron tunneling, which can unlock the full potential of applications with high scientific and societal impact, including molecular electronics, [4][5][6][7][8][9] quantum tunneling, [10,11] plasmonic nano-optics, [12][13][14][15][16][17] and highly sensitive sequencing. [18][19][20] Despite their importance, fabrication of sub-5 nm NGEs remains a great technological challenge. [1] Existing NGEmanufacturing methods can be typically classified into two strategies: physical methods based on planar nanofabrication techniques and chemical methods based on noble metal nanoparticles. Most chemical methods are suitable for creating sub-1 nm NGEs [11][12][13][14][15] but limited to a relatively narrow range of applications owing to the contamination induced by linker molecules, the shell-filled gaps, and/or the restrictions derived from metal nanoparticle size. Physical methods, including direct patterning techniques, [21][22][23] breaking-/cracking-based methods, [6][7][8][9][10][16][17][18][19][20][24][25][26][27][28] and controllable deposition, [29][30][31] are fundamentally limited by the basic planar nanofabrication techniques. Particularly, direct patterning techniques variously suffer from high equipment costs, low throughput, and poor scalability to large sizes. The breaking-/cracking-based methods are the most widely used but typically involve direct patterning techniques to predefine the wire pattern, a complex apparatus to induce external stimuli, or special materials (e.g., brittle films) to induce internal stress. Though breaking-based methods can be used to produce sub-1 nm NGEs, [6][7][8][9][10][16][17][18][19][20] the intrinsic obstacles mentioned above result in discrete and material-limited NGEs with the fractal facing electrode surface blocking the realization of large-scale complex systems. Controllable deposition [29][30][31] is relatively simple for large-scale fabrication, while the formed NGEs typically face limitations derived from large gap width, problematic rough surfaces, the solution environment, or/and contaminations from the shadow-mask fabrication process. However, simply continuing to improve existing NGE-fabricating methods is insufficient since each method has its own serious inherent defects. An innovative approach is urgently needed to address these issues and to promote the developments of NGEs-based applications.Here, we demonstrate macroscopically measurable and material-independent NGEs with angstrom-scale separations Nanogap electrodes (NGEs) with decreasing separations have received growing attention due to their potential in stimulating extensive applications with high scientific impact, including molecular electronics, quantum tunneling, plasmonic optics, and highly sensitive sequencing. Although various NGE-manufacturing methods have been developed and offer promising results, angstrom-scale NGEs have not been achieved without requiring sophisticated equipment, restricting materials or substrates, compromising mass-fabric...