By combining a three-component reaction of 2, 3-diaminomaleonitrile, ketones and isocyanides with a subsequent reaction of 1,6-dihydropyrazine-2,3-dicarbonitrile derivatives obtained from isocyanide-based three-component reaction with various alkyl and aryl isocyanates or isothiocyanates can be assembled a new class of highly substituted imidazo[1,5-a]pyrazine derivatives.