The zwitterionic compounds 1-(diaminomethyleneammonio)(aryl)methyl-4,4-dimethyl-2,6-dioxocyclohexan-1-ides were synthesized from the reaction of dimedone, aromatic aldehydes and guanidine carbonate catalyzed by NaOH under solvent-free conditions. This is the new type azomethine ylide compound that has not been reported previously. The other advantages of this reaction were simple operation, short reaction time, and environmental friendly. The products were identified by 1 H NMR, 13 C NMR, IR and HRMS, and that of 4a was additionally confirmed by X-ray diffraction analysis. This reported approach is an effective way for the synthesis of azomethine ylide.