β-NiAl coatings on a superalloy substrate will inevitably result in severe rumpling at elevated temperatures; however, the associated rumpling mechanisms are not completely understood. The scale rumpling behavior of a β-NiAlHf coating deposited by electron beam physical vapor deposition (EB-PVD) on single crystal superalloy IC21 was investigated in this work. Some internal factors, including the mismatch in the coefficient of thermal expansion and the stress induced by the growth of oxide scale and the phase transformation, were taken into consideration. The thermal mismatch stress between the coating and substrate was the main internal factor responsible for rumpling behavior during thermal cyclic loads, while the phase degradation from β-NiAl to γ’-Ni3Al in the coating played a dominant role during static thermal loads.