To improve the economics of commercial nuclear power production, utilities are seeking to increase the allowable burnup limit of UO 2 fuel. One of the main factors that contributes to the current burnup limit of 62 GWd/MTU in commercial light-water reactors (LWRs) is the risk of fine fragmentation or pulverization during a loss of coolant accident (LOCA). Pulverization primarily occurs at high burnups, especially when the high-burnup structure (HBS) has formed. To allow the industry to pursue increased burnup and develop mitigation strategies, it is essential to have improved capability to predict the onset of pulverization. However, the mechanism of pulverization is not well understood, and the existing predictive capabilities implemented in the BISON fuel performance code are empirical in nature.In this report, mesoscale simulations are used to improve understanding of the formation mechanism of the HBS and how it responds during a LOCA transient, and inform development of a BISON pulverization criterion. A phase-field model was used to simulate the evolution of bubble pressure as a result of HBS formation. The simulations showed that gas atoms diffuse from grain interiors to the new grain boundaries created during HBS formation and diffuse rapidly along these grain boundaries to reach existing bubbles. This causes an increase in bubble pressure in existing bubbles, leading to bubble growth during steady-state operation. To simulate the response of HBS bubbles to a LOCA transient, a newly developed phase-field model was used; in agreement with preliminary results from Fiscal Year 2020, bubble size did not change significantly during the duration of the transient. A phase-field fracture model was used to study fragmentation patterns in the HBS. Phase-field fracture simulations were used to determine a pulverization criterion for BISON. A function for the critical pressure for pulverization to occur was fit to data from the phase-field fracture simulations, and this function was implemented as a material property in BISON. For comparison, an analytical criterion for pulverization was developed and implemented within the same material property.