In this paper, we synthesized 10 to 20 nm diameter NiFe nanoparticles and nanoparticle films utilizing supersonic jet deposition of nanoparticle aerosols generated by laser ablation of $30;to;45{mu}m$ diameter permalloy $(Ni_{81}Fe_{19} ;at;{\%})$ microparticles. The component and composition of the nanoparticles were characterized by an energy dispersive X-ray spectroscopy. The morphology of the nanoparticles and nanoparticle films was analyzed by a high-resolution transmission electron microscopy and a scanning electron microscopy, respectively. The experimental results showed that the nanoparticles and nanoparticle films have remarkable properties with an excellent preservation of the composition of feedstock permalloy microparticles. The purpose of the present work is to present details on the composition and nanostructural characterizations for NiFe nanoparticles and nanoparticle films prepared by laser ablation of microparticles (LAM).