Mössbauer spectra of 57Fe in the nickel–zinc ferrite system (ZnO)x(NiO)1−xFe2O3 have been obtained, at room temperature and at 77 °K, in zero magnetic field and also in a longitudinal magnetic field of 13.5 kG, covering the full range of zinc content. The dependence of the isomer shifts, line widths, quadrupole interactions, and nuclear magnetic fields of 57Fe3+ ions in both tetrahedral and octahedral sites has been determined. The principal results of this study are (a) the confirmation of the determination of the nuclear magnetic fields by Abe et al. using NMR, and the extension of these measurements to higher zinc concentrations, (b) an indication that the hypotheses of paramagnetic centers, proposed by Gilleo, and superparamagnetic clusters, proposed by Ishikawa, are not applicable to the nickel–zinc ferrites, (c) evidence of canted spin structures, first proposed by Yafet and Kittel, (d) various effects of chemical disorder in the nickel-zinc ferrites, and (e) an observation of the effect on the Mössbauer spectrum of relaxation in a magnetically ordered iron system.