Structural and magnetic properties of nanocrystalline Ni0.65Zn0.35Fe2O4 synthesized by sol-gel method have been analyzed using various characterization techniques. The single-phase spinel structure and crystallite size have been obtained from X-ray diffraction (XRD). The experimentally observed high specific saturation magnetization, 176 emu/g at 10 K, has been discussed in terms of core-shell contributions based on spin canting of nano Ni0.65Zn0.35Fe2O4 with the help of infield Mössbauer study at 5 K. The proposed cation distribution relied upon infield Mössbauer spectra and the Rietveld analysis of the neutron diffraction and XRD data and provides an insight to improve the properties of this material suitable for high-frequency applications.