Molecular beam epitaxy and scanning tunneling microscopy (STM) patterning are combined to form highly doped, planar devices in silicon at the atomic level. The absolute device location is registered to microscopic markers (see image; scale bar: 50 μm) for the alignment of surface contacts, enabling the correlation of the electrical properties of atomically controlled devices such as nanowires, tunnel junctions, and nanodots to the dopant location, monitored using high‐resolution STM techniques.