Intermetallic clusters are observed in the Co-Cr system. We report on the use of time of flight mass spectroscopy to investigate the cluster spectrum resulting from Nd-YAG ablation of a CoCr target. Cr + clusters dominated the spectrum, with Co + clusters as the second most intense peak, and we found a clearly resolved Cr-Co binary cluster that could be suitable for co-doping during the growth of laser crystals. Significant contributions from elemental dimers as well as some oxide clusters were also observed. Density functional calculations indicated that formation of the observed intermetallic clusters was thermodynamically favorable.