The structural parameters, exchange splittings, half-metallic property, electronic features and magnetic performances of Ba_1−xCr_xS materials were determined by utilizing the computational methods of density functional theory. The localized magnetic spins in the Ba_1−xCr_xS result from the effect of the hole carriers caused by the d shells of Cr atom, hybridizing with p levels of S atom. The ferromagnetism is mostly endorsed by the exchange splitting owing to its large contribution than that of the crystal field. The Ba_1−xCr_xS (x = 0.25), Ba_1−xCr_xS (x = 0.5)and Ba_1−xCr_xS (x = 0.75) materials have half-metallic characteristic with ferromagnetic state, where their electronic structures demonstrate spin polarizations of 100% with half-gaps of 0.815, 0.912 and 0.72 eV, respectively. Therefore, Ba_1−xCr_xS systems have better magneto-electronic performances, making them appropriate half-metallic materials for spin-injection applications for spintronics.