We propose that domain inversion can be directly induced by femtosecond laser both theoretically and experimentally, which opens a path to achieve three-dimensional (3D) nonlinear crystal with a period in sub-micron-scale. A simulation of domain inversion is modeled by considering the temporal distribution of femtosecond pulses. The calculation results clarify that the domain inversions can happen within or after the interaction with the laser pulse, and the response time of domain inversion is in the picosecond level depending on the intensity and the materials. The domain reversal windows of lithium niobate by femtosecond laser are observed which agrees with theoretical predictions qualitatively.