Abstract The synthesis of heterocyclic thioureas from heterocyclic amines with phenyl-or methylisothiocyanate or CS 2 is described. Seven new X-ray crystal structures are reported: In N-(3-pyridyl)-N′-phenylthiourea (P na2 1, a= 10.1453 (3), b= 17.6183 (5), c= 6.4787 (2), V= 1158.02 (6), Z= 4) hydrogen-bonding results in formation of a 3D network consisting of helices, which form channels parallel to the c-axis. In N-(4-pyridyl)-N′-phenylthiourea (P ...