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Its formation from ammonia and carbon dioxide requires either high pressures and temperatures or, under milder conditions, catalysts or additional reagents. In this study, we observed the spontaneous formation of urea under ambient conditions from ammonia and carbon dioxide in the surface layer of aqueous droplets. Single, optically trapped droplets were probed by using Raman bands as markers. We found the surface layer to act like a microscopic flow reactor, with chemical gradients providing access to unconventional reaction pathways. This observation revealed a general mechanistic scheme for distinctive droplet chemistry. 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