The 41 novel acylthiourea derivatives with hydantoin were synthesized in moderate to excellent yields by using 5-(4-aminophenyl)- and 5-(4-aminobenzyl)- hydantoin or 5-(4-aminobenzyl)-thiohydantoin as raw materials and characterized by IR, H-1 NMR spectra and elementary analysis. The preliminary bioassay showed that these compounds exhibit certain selectively herbicidal activities with the 91%, 94% and 87% inhibition rates of 7l, 8o and 8p against B. campestris, 100%, 100% and 95% efficacy against B. campestris in a greenhouse test, respectively. 7a, 7b, 7c and 7d exhibited 74%, 79%, 79% and 71% inhibition rates against F. oxysporum, respectively.