Abstract Reactions of 2-aminopicolines with 2-and 4-tolyl isothiocyanates yielded N-2-(4- picolyl)-N′-4-tolylthiourea, 1, N-2-(3-picolyl)-N′-4-tolylthiourea, 2, and N-2-(4-picolyl)-N′- 2-tolylthiourea, 3. Compound 1 is monoclinic, of space group P 2 1/c with a= 7.456 (1) Å, b= 13.135 (3) Å, c= 13.959 (3) Å, β= 104.99 (3)°, and V= 1320.5 (5) Å 3 with Z= 4, for d calc= 1.294 g/cm 3. Compound 2 is triclinic, of space group P ̄ 1 with a= 6.877 (3) Å, b= 7.590 ( ...