N-tosylimines have been successfully synthesized for the first time by condensations of N-tosylamine with aldehydes catalyzed by HY3, HY6, HY9 and HZSM-5 zeolites. HY9 was the best catalyst, leading to the highest yield of N-tosylimines, indicating that the reaction efficiency depends upon the concentration of the Bronsted acid sites and its hydrophobicity.