Stimulated by strong demand for thermal expansion control from advanced modern industries, various giant negative thermal expansion (NTE) materials have been developed during the last decade. Nevertheless, most such materials exhibit anisotropic thermal expansion in the crystal lattice. Therefore, strains and cracks induced during repeated thermal cycling degrade their performance as thermal-expansion compensators. Here we achieved giant isotropic NTE with volume change exceeding 3%, up to 4.1%, via control of the electronic configuration in Sm atoms of SmS, (4 f)6 or (4 f)5(5d)1, by partial replacement of Sm with Y. Contrary to NTE originating from cooperative phenomena such as magnetism, the present NTE attributable to the intra-atomic phenomenon avoids the size effect of NTE and therefore provides us with fine-grained thermal-expansion compensators, which are strongly desired to control thermal expansion of microregions such as underfill of a three-dimensional integrated circuit. Volume control of lanthanide monosulfides via tuning of the 4 f electronic configuration presents avenues for novel mechanical functions of a material, such as a volume-change driven actuator by an electrical field, which has a different drive principle from those of conventional strain-driven actuators such as piezostrictive or magnetostrictive materials.