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27 Al and 63.65Cu NMR measurements are reported for powder samples of stable Al-Cu-Fe and Al-Cu-Ru icosahedral quasicrystals and their crystalline approximants, and for an Al-Pd-Mn singlegrain quasicrystal. Furthermore, 27Al NQR spectra at 4.2 K have been observed in the Al-Cu-Fe and Al-Cu-Ru samples. From the quadrupole-perturbed NMR spectra at different magnetic fields, and from the zero-field NQR spectra, a wide distribution of local electric-field gradient (EFG) tensor components and principal-axis-system orientations was found at the Al site. A model EFG calculation based on a 1/1 Al-Cu-Fe approximant was successful in explaining the observed NQR spectra. The average local gradient is largely determined by the p-electron wave function at the A1 site, while the width of the distribution is due to the lattice contribution to the EFG. Comparison of 63CU NMR with 27Al NMR shows the EFG distribution at the two sites is similar, but the electronic contribution to the EFG is considerably smaller at the Cu site, in agreement with a more s-type wave function of the conduction electrons. The overall spread of EFG values is well reproduced by the calculation based on the approximant. However, the experimental spectra indicate a much larger number of nonequivalent sites when compared with the simulated NQR spectra based on the 1/1 approximant. The short-range, local chemical order is well represented by the approximant, but differences in coordination must be included at intermediate range in the quasicrystal. Measurements of 27Al Knight shift, magnetic susceptibility, and nuclear spin-lattice relaxation time as a function of temperature yield results which indicate a reduction of the density of states at the Fermi level by a factor of 7 or 8 from the value in Al metal, consistent with the notion of a pseudogap for these quasicrystals. No differences in the measured parameters were detected as a function of composition of the quasicrystatline alloys, arguing against a fine structure in the density of states at the Fermi level.