In this freshly published article, AFM is used to investigate the interplay between organic ligands and substrates during the crystallization of metal-organic frameworks (MOFs). In-situ AFM experiments were performed by TappingMode on a Bruker MultiMode AFM in aqueous solutions continuously flowing through the liquid cell at 30°C and 60°C. This allowed the research team at Pacific Northwest National Laboratory (PNNL) to visualize the kinetics of dissolution pits and extract nucleation and growth rates. Imaging forces were kept low (~50 pN) to ensure that there was no measurable effect of the AFM tip on the particle number density and growth kinetics. The experiments showed that a specific linker-step and linker-terrace interaction is due to energetically favorable configurations. These specific interactions lead to a deterministic means of controlling the dissolution kinetics of a substrate and therefore the growth kinetics of the outer layer.