The possibility of binary hard-sphere colloids crystallizing with the cesium chloride (CsCl) structure was examined experimentally using poly (methyl methacrylate) particles dispersed in organic solvents. Towards this end, two dispersions were prepared that contained particles with a radius ratio alpha=R(B)/R(A), where A refers to the large particles and B the small, of 0.736. This is close to the optimum ratio of 0.732 at which this structure is predicted to form as determined by space-filling calculations. The phases found within the binary mixture were examined using laser light crystallography and scanning electromicroscopy, and some were shown to have the CsCl structure. Over a period of time some of the CsCl crystals disappeared indicating that they were metastable and that this structure may not be the most enduring phase at this size ratio.