The system V(x)CrS2 (0 < x =1) has been investigated by X-ray and neutron powder diffraction. Five single-phase regions have been identified. All single-phase materials adopt pseudolayered structures, in which octahedral sites between alternate pairs of close packed sulfide layers are fully and partially occupied by cations. With increasing vanadium content, rhombohedral M2S3, trigonal M2S3, monoclinic M3S4, trigonal 3C-M7S8, and hexagonal M(1-x)S structures are successively observed. All single-phase materials exhibit semiconducting behavior, consistent with a variable range hopping conduction mechanism. Magnetic properties show considerably greater variation. The phase with the lowest vanadium content (rhombohedral M2S3) exhibits ferrimagnetic ordering at 100(10) K. Phases with higher vanadium content also exhibit long-range magnetic ordering, with the exception of the monoclinic M3S4, which is a spin glass (T(g) = 40(5) K).