A simple and efficient method has been developed for the synthesis of N-allylthioureas from allylic bromides in one-pot by using a supported reagents system, KSCN/SiO2– RNH3OAc/Al2O3, in which allyl bromide reacts first with KSCN/SiO2 and the product, allyl isothiocyanate, reacts with RNH3OAc/Al2O3 to give the final product, N-allylthiourea, in good yield.