Ultrafast　laser　lift-off　is　an　important　step　in　manufacturing　flexible　electronic　display　devices.　To　improve　the　picosecond　laser　lift-off　transfer　quality　of　micro　light　emitting　diodes　(micro-LEDs),　the　response　surface　methodology　(RSM)　is　employed　for　the　optimization　of　multiple　laser　processing　parameters,　including　laser　power,　scanning　speed,　spot　diameter,　and　scanning　distance.　Transfer　yield　and　residual　stress　are　chosen　as　the　performance　evaluation　metrics,　as　well　as　the　lifted-off　device　element　composition　and　transfer　quality　under　different　process　parameters　are　characterized.　The　optimized　maximum　transfer　yield　is　95.84%　and　the　minimum　residual　tensile　stress　is　0.589　GPa,　which　is　less　than　0.5%　prediction　error　of　the　optimum　transfer　yield　(95.67-95.74%)　and　residual　stress　(0.588-0.592　GPa)　for　ultrafast　laser　lift-off　of　micro-LEDs　based　on　the　central　composite　design　of　RSM,　indicating　the　reliable　guidance　ability　of　this　model.　It　develops　a　new　way　for　quality　improvement　of　the　ultrafast　laser　lift-off　process　for　micro-LEDs.