The surface profile of laser peening with square spots was compared with that of circle spots, and the microstructure of laser peened titanium alloy Ti-6Al-4V in the center of a square spot and at the edge of the square spot was investigated in this paper. The results show that a smaller size crystal is produced at the edge of square spots because the shearing strain produces nanoscale crystals in laser peening titanium alloy Ti-6Al-4V.