The purpose of the study was looking for the novel compounds with herbicidal activities. Intermediate 4-(4,6-dimethoxypyrimidin-2-yloxy)-2-methylbenzaldehyde(3) was synthesized using m-cresol as starting material by acylation reaction and substitution reaction. Twelve novel 2-(4-(4,6-dimethoxypyrimidin-2-yloxy)-2-methylphenyl)-2-(substituted phenylamino) acetonitrile derivative compounds have been synthesized using intermediate (3) via three component one-pot reaction, and the yields are 64～96%. The structures of all synthesized compounds were confirmed by 1H NMR, MS and elemental analysis techniques.