Magnetic, nano-crystalline samples of zinc substituted nickel ferrite, (Zn x Ni 1-x Fe 2 O 4 for x = 0.0-0.9 in step of 0.2), are synthesized using microwave combustion synthesis technique. The structural properties of Ni-Zn are determined using X-ray powder diffraction, transmission electron microscopy; Fourier transforms infrared spectroscopy and neutron diffraction techniques. Average crystalline size obtained from X-ray diffraction and neutron diffraction is in the range of 30-60 nm. The cation distribution obtained from X-ray diffraction and neutron diffraction show that Zn occupies only tetrahedral A-site in the spinel lattice. The values of magnetic moment derived from magnetization measurements and neutron diffraction agrees nearly 97 % to that of bulk at 300 K. This methodology can be used to prepare large quantities (about 10 g) of sample at one time using kitchen microwave oven working at 1,200 W power.