Permalloy (Ni81Fe19) nanoparticles with diameters of hundreds of nanometers have been successfully fabricated by pulsed laser ablation (PLA) in air, distilled water, pure ethanol and sodium dodecyl sulfate (SDS) aqueous solutions. The permalloy nanoparticles made in SDS solutions are typically spherical in shape. Lower laser energy with lower frequency leads to the formation of smaller permalloy nanoparticles. Higher concentration of SDS results in smaller nanoparticles. Lastly, we found some unusual permalloy nanoparticles with interesting morphologies made by PLA in air, distilled water and ethanol.