The present disclosure provides a method of an ultrafast-pulsed laser deposition and a device thereof, wherein a single emitted femtosecond pulse is split, and the split pulses are synchronized in the time domain, and then coupled with each other to form a plasma grating or lattice to excite the target material once; then multiple pulsed lasers are sequentially coupled multiple times with the plasma gratings or lattices to excite the target material multiple times, and the excited target material is deposited and reacted on the substrate to form a thin film.