Giant Mine, an abandoned gold mine near Yellowknife in the Northwest Territories of Canada, generated significant arsenic trioxide roaster waste (ATRW) during its operations, posing a substantial environmental hazard. This study explored the feasibility of stabilizing ATRW by incorporating it into cemented paste backfill (CPB). Using response surface methodology (RSM), CPB samples with varying mixing ratios were analyzed to identify key parameters influencing strength. Unconfined compressive strength (UCS) tests assessed physical stability, while saturated hydraulic conductivity and computed tomography (CT) analyses examined the microstructure of the CPB. The results revealed that CPB samples prepared with general use (GU) cement exhibited significantly higher strength than those with a GU and lime kiln dust (LKD) mixture. Binder and solid contents were identified as the most critical factors influencing UCS, with binder content having a more pronounced influence. Curing time was found to be non-significant. Higher binder and solid contents correlated with higher UCS values in the CPB samples. The addition of 10% wt. ATRW reduced the UCS by over 30%, particularly in samples with lower binder and solid contents. Although microstructure differences were not evident in saturated hydraulic conductivity tests, CT scans showed increased formation of high-density arsenic-containing materials in samples with the highest UCS, especially those using GU binder. These findings suggest that optimizing binder and solid contents is crucial for enhancing CPB strength and effectively stabilizing ATRW.