Calcium sulfate (CS) is one of the oldest bone graft materials still in use. Its main limitations are poor handling characteristics, poor mechanical properties, and a resorption rate that is too fast for some applications. The present study investigated the effect of viscous polymers, such as carboxymethylcellulose (CMC) and hyaluronan (HY), on the handling characteristics, mechanical properties, and degradation behavior of CS. CMC and HY were added to CS at concentrations from 1-10 wt%. Addition of CMC to CS at more than 4 wt% produced a putty-like material and decreased the density of the composite, while also increasing flexural and compressive strength at higher loadings. Incorporation of CMC produced a concentration-dependent increase in water absorption and degradation rate. At an equivalent loading, HY-containing CS composites showed better compressive strength than CS with CMC. Overall, addition of CMC or HY to CS resulted in composite materials with better handling characteristics and improved mechanical properties after set, however the degradation rate of the augmented materials was increased. These properties suggest that the enhanced CS materials may be useful in certain clinical situations, such as filling non-uniform bone defects and situations that require mechanical integrity of the bone graft substitute during implantation.