Palladium　nanosheets　(Pd　NSs)　are　widely　used　as　electrocatalysts　due　to　their　high　atomic　utilization　efficiency,　and　long-term　stability.　Here,　the　electronic　structure　modulation　of　the　Pd　NSs　is　realized　by　a　femtosecond　laser　irradiation　strategy.　Experimental　results　indicate　that　laser　irradiation　induces　the　variation　in　the　atomic　structures　and　the　macrostrain　effects　in　the　Pd　NSs.　The　electronic　structure　of　Pd　NSs　is　modulated　by　laser　irradiation　through　the　balancing　between　Au-Pd　charge　transfer　and　the　macros-strain　effects.　Finite　element　analysis　(FEA)　indicates　that　the　lattice　of　the　nanostructures　undergoes　fast　heating　and　cooling　during　laser　irradiation.　The　structural　evolution　mechanism　is　disclosed　by　a　combined　FEA　and　molecule　dynamics　(MD)　simulation.　These　results　coincide　well　with　the　experimental　results.　The　L-AuPd　NSs　exhibit　excellent　mass　activity　and　specific　activity　of　7.44　A　mg-1　Pd　and　18.70　mA　cm-2　toward　ethanol　oxidation　reaction　(EOR),　4.3　and　4.4　times　higher　than　the　commercial　Pd/C.　The　2500-cycle　accelerated　durability　(ADT)　test　confirms　the　outstanding　catalytic　stability　of　the　L-AuPd　NSs.　Density　functional　theory　(DFT)　calculations　reveal　the　catalytic　mechanism.　This　unique　strategy　provides　a　new　pathway　to　design　the　ultrathin　nanosheet-based　materials　with　excellent　performance.　The　electronic　structure　modulation　of　the　Pd　NSs　is　accomplished　by　femtosecond　laser　irradiation　through　the　balancing　between　Au-Pd　charge　transfer　and　the　macros-strain　effects,　and　the　samples　exhibit　excellent　catalytic　performance　toward　EOR.　The　structural　evolution　and　the　catalytic　mechanisms　are　disclosed　theoretically.　This　strategy　provides　a　new　pathway　to　the　design　of　Pd　NSs-based　materials　with　excellent　performance.　image