Single crystals of Nd3ClS2[SiS4] were prepared from the. elements. Data collection was carried out using a STOE image plate detector at 293 K. The compound crystallizes in the orthorhombic space group Pnma with eight familiar units in a cell of dimension: a = 1240.3 (2), b = 1035.8 (2), c = 1616.4 (3) pm The corresponding residual (all data) for the refined structures is 3.45%. In the crystal structure, the chloride ions form chains along [010] with trigonal coordination by the lanthanide ions. The magnetic behavior of powdered crystals was interpreted by ligand field calculations where the influence of the ligand field was taken into account by applying the angular overlap model and magnetic exchange by the molecular field approximation. (C) 2002 Elsevier Science Ltd. All rights reserved.