This Perspective aims to inform the heterogeneous catalysis and materials science community about the recent advances in Time of Flight-Secondary Ion Mass Spectrometry (ToF-SIMS) to characterize catalytic solids by taking large model H-ZSM-5 zeolite crystals as a showcase system. SIMS-based techniques have been explored in the 1980-1990’s to study porous catalyst materials but, due to its limited spectral and spatiotemporal resolution, there was no real major breakthrough at that time. The technical advancements of SIMS instruments, namely improved ion gun design and new mass analyser concepts, nowadays allow for much more detailed analysis of surface species relevant to catalytic action. Imaging with high mass and lateral resolution, determination of fragment ion patterns, novel sputter ion concepts as well as new mass analysers (e.g. ToF, FTICR) are just a few novelties which will lead to new fundamental insight from SIMS analysis of heterogeneous catalysts. The Perspective article ends with an outlook towards instrumental innovations and their potential use for catalytic systems, others than zeolite crystals.