LnCrS 3 (Ln = La, Ce, Nd, Sm) with NH 4 CdCl 3 structure type were prepared in high pressure synthesis at 4 GPa, 1373 K for 2 h. Their orthorhombic lattice parameters were a = 0.787(2), b = 0.385(1), c = 1.334(3) nm for LaCrS 3 ; a = 0.776(4), b = 0.379(2), c = 1.316(7) nm for CeCrS 3 ; a = 0.769(2), b = 0.377(1), c = 1.306(4) nm for NdCrS 3 ; and a = 0.764(5), b = 0.374(2), c = 1.297(8) nm for SmCrS 3 . The Ln 3 + ions are coordinated with nine S 2 - ions in CrS 6 double chains. The products are antiferromagnetic semiconductors. The paramagnetic temperature Θ varied with a Cr-Cr distance in the CrS 6 double chain. They also showed a weak ferromagnetic behavior at low temperature below 120 K. Magnetic hysteresis was observed for the ferromagnetism between ZFC and FC measurements. LaCr 1 - x Fe x S 3 solid solution with NH 4 CdCl 3 structure type was also obtained in high pressure synthesis at 4 GPa, 1473 K for 2 h. The Fe 3 + in high spin state substitutes the Cr 3 + up to about x = 0.2.