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Deposition of aerosolized desert dust can affect marine microbial community structure and function through pulsed addition of limiting micro‐ and macronutrients. However, few studies have captured responses to dust deposition in situ following trans‐oceanic transport. We conducted a 26‐d time series evaluating biogeochemical and microbial community response to Saharan dust deposition in surface waters in the subtropical western Atlantic (Florida Keys National Marine Sanctuary, U.S.A.). Following periods of elevated atmospheric dust concentrations, particulate and dissolved iron concentrations increased in surface waters. Autotrophic picoeukaryote abundance increased rapidly, followed by increases in the abundance of heterotrophic bacteria andSynechococcus. Concomitant to cell count changes, we observed successional shifts in bacterial community composition. The relative abundances ofProchlorococcusandPelagibacterdeclined with dust arrival, while relative abundance of heterotrophic bacteria increased, beginning with Vibrionales and followed sequentially by Chrysophyceae, Rhodobacteriaceae, and Flavobacteriaceae. Finally, a peak inSynechococcuscyanobacteria was observed. These results provide new insight into microbial community succession in response to Saharan dust deposition, their association with temporal dynamics in surface water dissolved and particulate iron concentrations, and a potential role for bioprocessing of dust particles in shaping marine microbial responses to deposition events.