Several samples of CrSxwith 1.145<x<1.200 were carefully prepared and chemically analyzed. The expected crystal structures were verified by x‐ray analysis, which failed to indicate the presence of any impurities. Conductivity measurements indicated the existence of metallic conductivity in these samples between 77° and 300°K. Magnetic measurements supported the suggestion that the ferrimagnetism of CrSxmaterials arises from the presence of the Cr5S6phase.The magnetization curves forx=1.194 demonstrated the following salient properties of the Cr5S6phase: a ferrimagnetic Curie point of 305°K, a peak magnetization of 6.9 emu/gm in an external field of 8500 oe, a ferrimagnetic‐antiferromagnetic transition over a 5° temperature interval, a transition temperature in the neighborhood of 158°K which is subject both to thermal hysteresis and to shifting by an external magnetic field, and an antiferromagnetic susceptibility below this transition. The transition temperature, as well as the peak magnetization, decreases with increasing chromium content. A simple model is tentatively proposed, and appears to be consistent with the observed behavior.