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Here we developed a microdroplet-based strategy for the rapid synthesis of uniform polydopamine nano- and microspheres. Polydopamine spheres with controllable sizes were generated within hundreds of microseconds by simply spraying water solutions of dopamine into microdroplets. Mass spectrometry revealed that dopamine was primarily oxidized into aminochrome, acting as the major building block for polydopamine. We anticipate that microdroplet chemistry will be rich in opportunities for the synthesis of functional nano- and micromaterials. [ABSTRACT FROM AUTHOR]