Four urea derivatives were isolated from the roots of Pentadiplandra brazzeana, and their structures were elucidated by spectroscopic techniques. N-Benzyl-N′-(4-methoxybenzyl)urea (1) is a new compound, although N,N′-di-(4-methoxybenzyl)urea (2), N,N′-dibenzylurea (3), and p-methoxythiobenzaldehyde (4) are reported from a natural source for the first time.