Twenty four novel 2-benzylsulfonyl-5-methyl-1,2,4-triazolo[1,5-a]pyrimidine-7-oxoacetohydrazone derivatives 5a~5x were synthesized by utilization of 2-benzylthio-5-methyl-7-hydroxyl-1,2,4-triazolo[1,5-a] pyrimidine as starting material. All the target compounds were characterized by 1 H NMR, IR, MS and elemental analysis. The preliminary bioassay indicated that the inhibition rates of 4-methoxybenzaldehyde N- [2-benzylsulfonyl-5-methyl-1,2,4-triazolo[1,5-a]pyrimidine]-7-oxoacetohydrazone (5k), 2-choro-5-nitrobenzaldehyde N- [2-benzylsulfonyl-5-methyl-1,2,4-triazolo[1,5-a]pyrimidine]-7-oxoacetohydrazone (5p) and cinnamaldehyde N- [2-benzylsulfonyl-5-methyl-1,2,4-triazolo[1,5-a]pyrimidine]-7-oxoacetohydrazone (5s) against Botrytis cinerea reached above 70% at the concentration of 50 μg/mL.