Magnetoelectric (ME) film composites consisting of piezoelectric and magnetostrictive materials are promising candidates for application in magnetic field sensors, energy harvesters, and ME antennas. Conventionally, high‐temperature annealing is required to crystallize piezoelectric films, restricting the use of heat‐sensitive magnetostrictive substrates that enhance ME coupling. Herein, a synergetic approach is demonstrated for fabricating ME film composites that combines aerosol deposition and instantaneous thermal treatment based on intense pulsed light (IPL) radiation to form piezoelectric Pb(Zr,Ti)O3 (PZT) thick films on an amorphous Metglas substrate. IPL rapidly anneals PZT films within a few milliseconds without damaging the underlying Metglas. To optimize the IPL irradiation conditions, the temperature distribution inside the PZT/Metglas film is determined using transient photothermal computational simulation. The PZT/Metglas films are annealed using different IPL pulse durations to determine the structure–property relationship. IPL treatment results in an enhanced crystallinity of the PZT, thus improving the dielectric, piezoelectric, and ME properties of the composite films. An ultrahigh off‐resonance ME coupling (≈20 V cm−1 Oe−1) is obtained for the PZT/Metglas film that is IPL annealed at a pulse width of 0.75 ms (an order of magnitude higher than that reported for other ME films), confirming the potential for next‐generation, miniaturized, and high‐performance ME devices.

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