Sculpting 2D Nanosheet Architectures via Predictive Low‐Field Magnetic Alignment

ABSTRACT Controlling the macroscopic assembly of two‐dimensional (2D) nanosheets into functional, ordered architectures is a central challenge in materials science. Their intrinsic tendency to restack into dense, disordered films severely limits their potential in applications requiring directional transport, from catalysis to energy storage. Aligning atomically‐thin nanosheets has remained a major hurdle, a failure previously ascribed to thermal motion but which we identify as stemming from dominant, many‐body van der Waals interactions creating deep kinetic traps. Here, we overcome this barrier with a magnetic strategy enabling predictive architectural control at low field strengths (<50 mT). We establish a parameter‐matching model that deciphers the complex energy landscape, transforming assembly into a rational design framework. This approach allows us to sculpt architectures like vertically aligned, biaxially ordered MXene structures, creating ion superhighways with minimized tortuosity. As a demonstration, engineered MXene electrodes deliver exceptional rate capabilities in supercapacitors and sodium‐ion batteries. This work provides a universal, scalable platform for architecting 2D materials, unlocking their potential where directional transport is paramount.