CrS molecules Mere produced in a supersonic free jet expansion by reacting laser ablated chromium atoms and carbon disulfide. High-resolution laser-induced fluorescence spectrum between 625 and 825 nm was recorded. Six bands have been observed. which display the rotational structure of a Omega ' = - 1 - Omega " = -1 transition. Isotopic displacement analysis of (CrS)-Cr-52 and (CrS)-Cr-53 confirms that these six bands form a vibrational progression in a single band system. Ab initio calculations yielded spectroscopic properties of the two low-lying (5)Pi states: X(5)Pi (11 sigma (1)5 pi (1)1 delta (2)) and B(5)Pi (12 sigma (1)5 pi (1)1 delta (2)). From the good agreement between calculated and measured spectroscopic properties, we assign the observed transition as the B(5)Pi (-1)-X(5)Pi (-1).