Thin films of 3 different thicknesses each of Ni83.2Fe3.3Mo13.5 and Ni83.1Fe6.0Mo10.9alloys have been grown using Pulsed Laser Deposition (PLD) technique. Our motivation is to investigate the magnetic properties of a few nm thick Ni alloys with mostly Mo (4d element) addition since the corresponding soft ferromagnetic bulk alloys have shown very small coercivity of ˜ 0.1 Oe. Detailed structural characterization has been undertaken before probing the magnetic properties. Arc melted alloy buttons after homogenization are used directly as targets for the deposition. Films were deposited on single crystal Sapphire (0001) substrates using excimer laser. The structural characterization has been done by X-ray diffraction (XRD), X-ray reflectivity (XRR), Energy dispersive x-ray spectroscopy (EDS), and Atomic force microscopy (AFM). The X-ray diffraction pattern shows that the films are highly textured and grown along [111] direction of the alloys. They have high lattice strain which makes the films highly resistive and the resistance decreases with increasing thickness. The EDS measurements, using Scanning electron microscope (SEM), indicate that the compositions of the films are almost the same as those of the targets. Thickness, roughness, and density gradients are estimated using XRR measurements. The thinner films have higher roughness compared to the thicker ones for both the compositions. The films have density gradient across their thickness. The bottommost low density layer has high roughness which is supposed to be the result of initial non uniform coverage of the substrate. The density of the middle layer, having the lowest roughness, is approximately near the bulk value and it increases with increasing film thickness. The change in density is not due to the variation of composition; instead it is due to the variation of void densities in the layers. The topmost layer, having the lowest density and the highest roughness, is interpreted as a porous layer which is also evident from the AFM images.