We present first-principles computations of ferromagnetic electronic structures and spin-resolved Compton profiles along the three high-symmetry directions in Ni 75 Cu 25 and Ni 75 Co 25 disordered alloys, together with the corresponding Compton measurements from single-crystal specimens with a 137 Cs source. The theoretical results are based on the use of the charge-and spin-self-consistent Korringa-Kohn-Rostoker coherent-potentialapproximation framework to treat disorder, and the local spin-density scheme for incorporating exchangecorrelation effects; the lattice constants in all cases are obtained by minimizing the total energy. The majorityspin spectrum of Ni undergoes relatively small changes upon alloying with Cu or Co, and the associated majority-spin contribution to the Compton profiles of Ni, Ni 75 Cu 25 and Ni 75 Co 25 is nearly the same. In comparing theory and experiment, we focus on anisotropies in Compton profiles, and find the overall agreement with respect to the J 111 ϪJ 100 , J 111 ϪJ 110 , and J 110 ϪJ 100 anisotropies in Ni 75 Cu 25 as well as Ni 75 Co 25 to be reasonable, although some significant discrepancies around p z ϭ0 are notable. We show clearly that the momentum resolution of 0.4 a.u. ͑full width at half maximum͒ of the present experiment washes out some of the fine structure in the Compton spectra, and that these spectral features should be accessible via higher resolution measurements with a synchrotron light source.