The reliability of the flip chip package is strongly influenced by underfill, which has a much higher coefficient of thermal expansion (CTE) compared with other packaging materials and leads to large thermomechanical stresses developed during the assembly processes. Thermal expansion mismatch between different materials causes interface delamination between epoxy molding compound and silicon die as well as interface delamination between underfill and silicon die. The main objective of this study is to investigate the effects of underfill material properties, fillet height, and silicon die thickness on the interface delamination between epoxy molding compound and silicon die during a lead-free solder reflow process based on the modified virtual crack closure method. Based on finite element analysis and experiment study, it can be concluded that the energy release rates at reflow temperature are the suitable criteria for the estimation of interface delamination. Furthermore, it is found that underfill material properties (elastic modulus, CTE, and chemical cure shrinkage), fillet height, and silicon die thickness can be optimized to reduce the risk of interface delamination between epoxy molding compound and silicon die in the flip chip ball grid array package.