Ni1−xZnxFe2O4 nanoparticles (x = 0.0–1.0) were successfully prepared via sucrose-assisted autocombustion method. Thermal analysis measurements indicated that the ferrite nanoparticles could be synthesized in this self-propagating combustion process. The microstructure and magnetic properties were investigated by means of X-ray diffraction, transmission electron microscope, Fourier transform infrared, and vibrating sample magnetometer. The crystallite sizes obtained using Scherrer’s equation are in the range 25–35 nm. An appropriate cation distribution was suggested based on the structural and magnetic measurements. The increase in the saturation magnetization with increasing Zn-content up to x = 0.4 and its subsequent decrease was discussed in the view of entire cation distribution. The decrease in the coercivity with increasing Zn content was attributed to the change in the magnetocrystalline anisotropy.