The ultra-high plastic deformation behavior by laser shock processing on the LY12 aluminum alloy had been investigated. The morphology of the materials had been analyzed by transmission electron microscopy (TEM) and scanning electron microscopy (SEM). It was found that the grain refinement layer was formed in the thickness of about 100μm .The dislocation density of LY12 aluminum alloy should be large increased after laser shocking because the accumulation of dislocation was appeared on the grain boundary. With the laser energy density increased there formed subgrain structure and eventually generate ultra-fine grain. Hardness test results also show that the surface hardness obtains a big growth about 60% after laser shock processing. The results showed that the formation of ultra-high plastic strain can improve the surface hardness of LY12 aluminum alloy, and thus effectively improve the comprehensive mechanical properties.