Structure and quality of ultrathin iron films on Cu(100) prepared by pulsed laser deposition (PLD) were studied by means of low electron energy diffraction (LEED). As in the case of thermal deposition (TD) the film undergoes a structural transition from a tetragonally expanded phase to the undistorted fcc structure at an iron coverage of 5 monolayers (ML). The changed structure of the Fe/Cu interface and the improved film quality are discussed in terms of the laser-fluence dependency of the deposited particle energies for PLD.