An increase in the remanence of an isotropic film magnet is indispensable to improve the properties of miniaturized devices. We, therefore, tried to prepare Pr–Fe–B/α-Fe multilayered nanocomposite thick-film magnets by a pulsed laser deposition (PLD) method. Namely, a rotated target composed of a Pr<inf>x</inf>Fe<inf>14</inf>B (x = 2.2 or 2.4) target together with an α-Fe segment was ablated. We also took account of a small spot size of the laser beam in order to suppress the emission of droplets (large particles) from each target. An optimization on the area of the α-Fe segment in each Pr<inf>x</inf>Fe<inf>14</inf>B target was carried out, and the remanence of an annealed film reached approximately 1.1 T. Moreover, a transmission electron microscopy (TEM) observation of the above-mentioned sample revealed that the microstructure varied from a multilayered structure (as-deposited) to a dispersed one through the annealing process. Resultantly, the annealed film had a dispersed nanocomposite structure with good exchange coupling.