This report provides a best-estimate evaluation of residual water content (post-dry out) in the High Burnup (HBU) LWR Spent Fuel Demonstration project TN-32 cask, and evaluates the radiolysis of the residual free water, and the physisorbed and chemisorbed waters on the surfaces of the fuel and cask internal contents. 1 The evaluation of radiolytic breakdown of those waters with gamma radiation causing the generation of hydrogen gas (H2) is made using available literature data and models. This evaluation is part of the overall materials performance evaluation of the SNF-in-canister system, and is part of the technical bases for their continued safe dry storage.The TN-32 cask contents included 32 HBU LWR spent fuel assemblies each with 264 fuel rods clad in zirconium alloys, aluminum neutron absorber components, and aluminum and stainless steel structural components. The residual free and surface (physisorbed/chemisorbed) waters are ascribed to water vapor in the free volume and to components' surfaces, respectively. The total potential radiolytic hydrogen inventory from the water vapor and from waters ascribed to surfaces has been calculated assuming all the water produced molecular H2. The residual water that is chemically incorporated into the bulk of a hydrated oxide, i.e., chemisorbed water, and its total potential hydrogen inventory has been calculated. These calculations are at the physical limit of material available and are used for a bounding assessment purpose only.An estimate was made of amount of hydrogen (H2) generated in the HBU cask free volume after 12 days and after 40 years with radiolysis of the residual waters. The oxygen from radiolytic breakdown of free and surface water (effective net reaction H2O = H2 + 1/2O2) is not built up in the canister, and rather is assumed to be consumed by oxidation reactions with the materials. The oxidation of materials in the canister, addressed in a previous report [Shukla et al, 2019] in the NE-SFWST campaign, is not discussed in this report. No oxygen (O2) generation is expected from radiolytic breakdown of chemisorbed water in hydrated oxides based on results of previous studies. Gettering of hydrogen and back reactions to reduce hydrogen concentration were not considered in this present work.