AbstractSoft ferromagnetic permalloy (NiFe) thin films are promising for applications in spintronic devices because of their constituent electrical and magnetic properties. Electron beam evaporation and sputtering techniques have been used to deposit NiFe thin films. For in situ stacking of NiFe with functional complex oxides, the pulsed laser deposition (PLD) method is highly desirable. However, the growth of high‐quality NiFe (and non‐oxide thin films in general) by PLD remains a formidable task. Here, high‐quality NiFe thin films of various thicknesses on oxide/non‐oxide substrates with desirable magnetic properties by PLD at room temperature are reported. The magnetic properties are found to be strongly dependent on the laser fluence of the deposition process. The laser fluence of 4 J cm⁻² produces the highest magnetization of ≈547 emu cc⁻¹. The small coercivity (few Oersted) and sharp ferromagnetic switching behavior indicate uniaxial anisotropy with an easy axis along the in‐plane direction. In addition, thickness‐dependent magnetodynamics characterizations are studied via ferromagnetic resonance. These results offer significant insight into the PLD‐based development of thin metal magnetic films.