The system of V 1−xTi xS 1.40 has been studied through magnetic susceptibility and NMR measurements. The Curie constant increases with quadratic dependence on the composition x within the V 3S 4 phase (0 ≤ x ≤ 0.6) and then, rapidly decreases toward the Ti 2S 3 phase (0.8 < x ≤ 1.0). The NMR absorption from V 51 nuclei with itinerant delectrons rapidly decreases with increasing Ti content in the former phase. These phenomena may indicate that local magnetic moments are formed in this system under a particular environment of vanadium atoms proposed. Metal distribution of V and Ti is also discussed.