Planar heterostructures composed of two or more adjacent structures with different materials are a kind of building blocks for various applications in surface plasmon resonance sensors, rectifiers, photovoltaic devices, and ambipolar devices, but their reliable fabrication with controllable shape, size, and positioning accuracy remains challenging. In this work, we propose a concept for fabricating planar heterostructures via directional stripping and controlled nanofractures of metallic films, with which self-aligned, multimaterial, multiscale heterostructures with arbitrary geometries and sub-20 nm gaps can be obtained. By using a split ring as the template, the asymmetric nanofracture of the deposited film at the split position results in nonreciprocal peeling of the film in the split ring. Compared to the conventional processes, the final heterostructures are defined only by their outlines, thus providing the ability to fabricate complex heterostructures with higher resolutions. We demonstrate that this method can be used to fabricate heterodimers, multimaterial oligomers, and multiscale asymmetrical electrodes. An Ag−MoS 2 −Au photodiode with a strong rectification effect is fabricated based on the nanogap heterostructures prepared by this method. This technology provides a unique and reliable approach to define nanogap heterostructures, which are supposed to have potential applications in nanoelectronics, nanoplasmonics, nanooptoelectronics, and electrochemistry.