“…The advantages conferred by nanowires have led to numerous advances in bottom-up synthetic routes, such as vapor- and solution-phase growth, − electrodeposition, − and lithographic methods, , which can yield freestanding magnetic nanowires with well-defined diameters, lengths, compositions, and phase purity. Challenges remain, however, because these traditional bottom-up methods often do not allow for precise control over the long-range nanowire morphologies, and they typically lead to surface passivation and the formation of defects. − Alternatively, one can employ top-down approaches to isolate wires from bulk crystals, as demonstrated with Mo 6 S 3 I 6 , − , SnIP, and V 2 Se 9 , , which comprise strong covalently bonded molecular chains connected by van der Waals (vdW) interchain interactions. This approach has shown great promise because starting from ostensibly more highly ordered and surface defect-free bulk crystals yields nanowires whose structural and physical properties enable potential applications in transistors and photovoltaic devices. ,− To our knowledge, however, these softer methodologies have not been extended to magnetic vdW phases and, critically, their utility in accessing highly desirable ultrathin magnetic nanowires remains largely unexplored.…”