Recently, we reported a PLD(Pulsed Laser Deposition)-fabricated isotropic nano-composite thick film magnets with dispersed α-Fe+Nd-Fe-B structure by using the laser energy density (LED) above 10 J/cm2  whose magnetic properties were superior compared with those previously reported α-Fe+Nd-Fe-B nano-composite films prepared by LED lower than 1 J/cm2 . However, the (BH)max value of a film prepared by LED蠇10 J/cm2 was inferior to those of isotropic RE (Nd or Pr)-Fe-B/α-Fe nano-composite ribbons with (BH)max above 130 kJ/m3 [3,4]. Furthermore, in order to apply the nano-composite films prepared by the high laser energy density to a miniaturized device, further enhancement in magnetic properties is required . An investigation on the formation of dispersed α-Fe + Nd-Fe-B structure is also indispensable to advance the preparation of a PLD-fabricated thick-film magnet. This contribution reports the improvement in (BH)max by controlling the film composition. In addition, the formation of microstructure of each film prepared by the high laser energy density was examined as a function of deposition time.