A novel assessment has been completed to determine the unquantified and uncredited safety margins (i.e., the difference between the licensing-basis and as-loaded calculations) available in as-loaded spent nuclear fuel (SNF) casks. This assessment was performed as part of a broader effort to assess issues and uncertainties related to the continued safety of casks during extended storage and transportability following extended storage periods. Detailed analyses crediting the actual as-loaded cask inventory were performed for each of the casks at three decommissioned pressurized water reactor sites to determine their characteristics relative to regulatory safety criteria for criticality, thermal, and shielding performance. These detailed analyses were performed in an automated fashion by employing a comprehensive and integrated data and analysis tool—Used Nuclear Fuel-Storage, Transportation and Disposal Analysis Resource and Data System (UNF-ST&DARDS). Calculated uncredited criticality margins from 0.07 to almost 0.30 keff were observed, calculated decay heat margins ranged from 4 to almost 22 kW (as of 2014), and significant uncredited transportation dose rate margins were also observed. The results demonstrate that at least for the casks analyzed here, significant uncredited safety margins are available that could potentially be used to compensate for SNF assembly and canister structural performance related uncertainties associated with long-term storage and subsequent transportation. The results also suggest that these inherent margins associated with how casks are loaded could support future changes in cask licensing to directly or indirectly credit the margins. Work continues to quantify the uncredited safety margins in the SNF casks loaded at other nuclear reactor sites.