Owing　to　the　increasing　energy　demands,　direct　small-molecule　fuel　cells,　such　as　ethanol　and　formate　fuel　cells,　have　attracted　great　attention.　During　the　operation　of　the　fuel　cell,　noble　metal　catalysts　are　widely　used　to　accelerate　the　reaction　kinetics　by　alloying　with　other　materials.　However,　there　are　a　few　facile　methods　for　improving　elemental　metal　catalytic　activity.　In　this　work,　the　defect-rich　palladium　(Pd)　aerogels　are　acquired　by　laser　ablating　technology,　which　can　significantly　improve　the　intrinsic　activity　of　Pd　elementary　catalysts　through　introducing　defects　and　lattice　strain.　The　electrochemical　results　show　that　the　mass　and　specific　activities　of　the　obtained　Pd　aerogel　for　the　formate　oxidation　reaction　are　2.26　and　1.99　times　higher　than　those　of　the　commercial　Pd/C.　The　excellent　activity　and　stability　of　the　Pd　aerogel　for　ethanol　oxidation　reaction　have　also　been　demonstrated.　The　effect　of　the　compressive　strain　is　further　investigated　by　density　functional　theory　(DFT)　calculations.　It　has　been　found　that　the　compressive　strain　weakens　the　adsorption　strength　of　the　intermediates,　which　can　facilitate　the　desorption　of　toxic　specifics.　The　laser-assisted　synthesis　of　defect-rich　aerogel　paves　a　way　in　optimizing　the　structure　of　the　elemental　metal　catalysts　and　improving　their　intrinsic　catalytic　activity.