As the need for smaller data storage devices in the market continues to grow, the study of new combinations of self-assembled magnetic nanoparticles/films is greatly needed. In this research, Fe50-Ni50 films were synthesized using a Pulsed Laser Deposition technique. The films were analyzed using scanning electron microscopy (SEM), atomic force microscopy (AFM) and physical properties measurement system (PPMS). Films were deposited from Fe-Ni alloy target (50%-50% composition), deposition was conducted in vacuum, at substrate temperatures varying from liquid nitrogen temperature -196°C to 600°C. The films were annealed in a vacuum chamber at 600°C for 1 hour. The study reveals that the substrate temperature has significant effect on the structure of the films and their magnetic properties. It was shown that additional thermal treatment improved the quality of films in terms of narrow grain size distribution. Magnetic properties were also found to improve significantly after post annealing process.