A simple, efficient and environment-friendly approach is described for the synthesis of N-alkyl-3,6-diaryl-[1,2,4]triazolo [4,3-b][1,2,4]triazin-7-amines based on three-component reaction between 5-aryl-4H-1,2,4-triazole-3,4-diamine, isocyanide and aldeyhde under solvent-free condition. The products are obtained in moderate to good yields and are in a state of high purity.