Binary Co-Cr alloys containing various Cr contents were vacuum induction melted and cast into wedge-shaped copper molds. It was intended to develop a microstructure (1) free from interdendritic segregation and porosity; (2) having minimal intermetallic precipitates; and (3) suitable for biomedical applications. The resultant microstructures were evaluated from sections obtained longitudinally and centrally in the plane normal to the diverging wedge faces. All ingots showed a dendritic microstructure with some characteristic features. For instance, in Co-20–30 wt. % Cr alloys, the chilled cast microstructures consisted of columnar dendrites without interdendritic segregation, a minimum of intermetallic precipitates, and the presence of a predominantly athermal HCP ε-martensite (>80 vol. %). In addition, the metastable FCC γ-Co phase was identified by X-ray diffraction and scanning electron microscopy. In the case of 35–44 wt. % Cr cobalt alloys, a eutectic constituent including the σ-phase were found to develop in the interdendritic regions. From this work, a Co-20 wt. % Cr alloy was chosen for further investigation after heat treating below the γ/ε transition temperature. The resultant tensile strength and ductility were further improved after applying a heat treatment at 730 °C for 30 min, obtaining values of elongation of 26% as compared with 2.55 < 5 of elongation in the as cast condition. Also, the alloy corrosion resistance in artificial saliva was investigated. It was found that the exhibited corrosion rates for the as-cast and heat-treated conditions are between those reported for other similar systems.