Twelve novel compounds of 1-substitutedphenyl-3-(5-halobenzimidazol-2-yl) acylurea were synthesized by the reaction of 5-halobenzimidazol-2-yl acylisocyanate with substituted anilines in yields of 62.4–76.1%. The structures of the title compounds were characterized by IR, 1H NMR spectra and elemental analysis. Antifungal activities against Botrytis cinerea and Sclerotinia sclerotiorum were also evaluated by the mycelium growth rate method in the lab. The results indicated that most of the title compounds exhibited excellent antifungal activities against Sclerotinia sclerotiorum, and their activities were higher than that of thiophanate-methyl.