Atomic layer deposition (ALD) is used to deposit 1-600 monolayers of Al2O3 on Ag nanotriangles fabricated by nanosphere lithography (NSL). Each monolayer of Al2O3 has a thickness of I A A. It is demonstrated that the localized surface plasmon resonance (LSPR) nanosensor can detect Al2O3 film growth with atomic spatial resolution normal to the nanoparticle surface. This is approximately 10 times greater spatial resolution than that in our previous long-range distance-dependence study using multilayer self-assembled monolayer shells. The use of ALD enables the study of both the long- and short-range distance dependence of the LSPR nanosensor in a single unified experiment. Ag nanoparticles with fixed in-plane widths and decreasing heights yield larger sensing distances. X-ray photoelectron spectroscopy, variable angle spectroscopic ellipsometry, and quartz crystal microbalance measurements are used to study the growth mechanism. It is proposed that the growth of Al2O3 is initiated by the decomposition of trimethylaluminum on Ag. Semiquantitative theoretical calculations were compared with the experimental results and yield excellent agreement.