Metal nanocatalysts are the workhorses of chemical industry and play a pivotal role in a vast set of chemical reactions. However, many catalysts deactivate during operation, e.g. by coke deposition or nanoparticle (NP) sintering, which comes with a high environmental and economic cost. To date, significant attempts have been undertaken to link the catalyst NP structure to its deactivation behavior via bulk characterization techniques. However, bulk averaging over all active site-types and NPs inherently blurs our vision when constructing robust structure-deactivation relationships. Herein, I propose a spatially-resolved characterization approach to decode catalyst deactivation at the single NP level and provide direct links to the NP structure. To this aim, model atomic layer deposition (ALD) based nanotailored Pt catalysts with target size and active site surface will be probed individually during and after propane dehydrogenation reaction and catalyst regeneration. In particular, super-resolution imaging by infrared, Raman and plasmonic nano-spectroscopy will be applied to follow-up on NP deactivation by coke deposition and sintering. This single particle approach, in general, will answer long-standing questions in metal nanocatalysis on the mechanisms of deactivation and produce guidelines for next-level catalyst design.