One of the challenges for the nanoscale device fabrication of III-V semiconductors is controllable postdeposition doping techniques to create ultrashallow junctions. Here, we demonstrate nanoscale, sulfur doping of InAs planar substrates with high dopant areal dose and uniformity by using a self-limiting monolayer doping approach. From transmission electron microscopy and secondary ion mass spectrometry, a dopant profile abruptness of ϳ3.5 nm/decade is observed without significant defect density. The n + / p + junctions fabricated by using this doping scheme exhibit negative differential resistance characteristics, further demonstrating the utility of this approach for device fabrication with high electrically active sulfur concentrations of ϳ8 ϫ 10 18 cm −3 .