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Serotonylation is a recently characterized PTM, wherein serotonin is covalently conjugated to glutamine residues of substrate proteins. This reaction is catalyzed by transglutaminases, and target substrates include small GTPases, fibronectin, cytoskeletal proteins, and histones. Serotonylation remodels the molecular functions of these proteins, thereby modulating diverse cellular signaling pathways and biological regulatory processes.