This report describes the synthesis of plutonium oxide (PuO2) samples at a bench-scale (10 g Pu) to support nuclear forensics research. The key unit operations that were performed included dissolving the PuO2 feed material, purifying the Pu by ion exchange, precipitating as plutonium (III) oxalate, and reconverting to PuO2 by calcination of the oxalate compound. Seventy-six PuO2 synthetic runs were performed in execution of a statistically designed test matrix. The process parameters varied in these synthesis runs included temperature (30 or 50 °C), the Pu concentration in the feed solution (10, 30, or 50 g Pu/L), the HNO3 concentration in the feed solution (1, 2, or 3 M), the direction of reagent addition (direct or reverse strike), the source of oxalic acid (solid or solution), and the reagent addition rate (as fast as possible, 20, or 40 minutes). This report describes the synthesis of the 76 PuO2 specimens. The characterization of these specimens will be described in separate reports.