Advanced manufacturing techniques offer tremendous potential in electronics, photonics, and biomedicine. Self‐assembly is a powerful strategy for creating three‐dimensional (3D) artificial structures, but existing thin film release techniques have limitations in the relatively complex processes. Herein, a localized laser scribing strategy is proposed to guide the self‐assembly of two‐dimensional thin films into 3D microstructures. It is revealed that laser‐induced heating and momentum can release thin films and roll them into various microstructures. Uniquely, this method allows accurate control of shapes, curvatures, orientations, and sizes for the fabricated rolls. This is a one‐step strategy with no pre‐patterning or post‐drying required. The proposed method represents a significant improvement over existing self‐assembly techniques and may enrich the thin film self‐assembly materials and applications. As proof of concept, the prepared gold micro‐rolls are demonstrated as implanted stents in porcine arteries with impressive flexibility. This study provides a new approach to creating 3D microstructures with simplicity and high repeatability and has significant implications for the future of advanced manufacturing, especially in emerging miniaturized applications, such as invasive robotics, minimized drug delivery, implanted batteries, and nanophotonics.