This work presents dicyanamide-containing ionic liquids as a new initiator system for cyanate ester resins. The cure effect was found in many dicyanamide-containing ionic liquids with diverse cations, and the dicyanamide was found to incorporate directly into the triazine network. The dicyanamide initiator provides an alternative to metal and hydroxyl catalysts, and produces a novel, ionic thermoset polymer. This polymer offers a new range of cure schedules, and opens the door to further research in degradation prevention, ionic thermosets, and nanocomposites. (C) 2016 Elsevier Ltd. All rights reserved.