High-resolution solid state Si-29, Al-27 magic angle spinning (MAS) and Al-27 triple quantum magic angle spinning (3Q-MAS) NMR spectroscopic techniques were used to characterize highly crystalline ultrastable Y (USY) zeolites having different framework Si/Al ratios, obtained by multistep-temperature-programmed (MSTP) steaming at different temperatures. The 29Si MAS NMR spectra of high silica USY show, in addition to the regularly ordered Q(4)(Si) framework sites (delta approximate to -105 ppm), the presence of distorted tetrahedral environments (delta approximate to -111 ppm), generated by the healing of the framework vacancies created by dealumination. Further, Al-27 MAS experiments show the presence of aluminum in four (Al-IV), five (Al-V), and six (Al-VI) coordinations, whereas the multiplicity within Al-IV and Al-VI is revealed by Al-27 3Q-MAS experiments. Two different tetrahedral and octahedral Al environments are resolved in the samples subjected to increasing steaming severity. Quantification of all the Al environments is provided based on isotropic chemical shifts (delta(CS)) and second-order quadrupole interaction parameters (P-Q), which were derived by a graphical analysis of 3Q-MAS data. In high silica USY materials prepared by MSTP method, the two Al-IV species resolved by 3Q-MAS experiments could be assigned to Al environments which are tetrahedrally connected to silicons in the original and healed regions of faujasite framework.