Some 4-N-(phenylamino)-6,7-methylenedioxy-quinazolines were synthesized from the commercially available 6-nitropiperonal, in good yields. This aldehyde was oxidized to the carboxylic acid, followed by reduction to the aminocarboxylic acid, which on condensation with formamidine acetate gave the corresponding quinazolinone. This was converted to its chloro-derivative, which by reaction with substituted anilines afforded the title compounds. All compounds were characterized by ¹H and ¹³C NMR, IR spectroscopy, MS spectral data and elemental analysis. The main goal for the synthesis of these compounds is their further pharmacological application, since it has been found that 4-anilinoquinazolines are potent and selective inhibitors of Epidermal Growth Factor receptor tyrosine kinase phosphorylation.