2D　Ni-Fe-MOF　ultrathin　nanosheets　(NSs),　with　dimensions　of　ca.　1.0　mu　m　and　thickness　of　ca.　5.0　nm,　were　successfully　fabricated.　Small-sized　Pd　nanoparticles　of　ca.　3.0　nm　were　deposited　on　2D　Ni-Fe-MOF　NSs　to　afford　Pd/Ni-Fe-MOF　NSs,　which　were　used　as　an　efficient　multifunctional　catalyst　to　realize　the　N-alkylation　reactions　of　amines　by　alcohols　under　visible　light.　The　superior　performance　observed　over　the　resultant　Pd/Ni-Fe-MOF　NSs　as　compared　with　Pd/bulk　Ni-Fe-MOF,　their　3D　counterpart,　can　be　ascribed　to　the　ultrathin　nanosheet　morphology　of　2D　Ni-Fe-MOF　NSs,　which　not　only　shortens　the　transportation　path　for　the　photogenerated　charge　carriers,　but　also　can　provide　more　efficient　interaction　between　the　active　site　and　substrates.　This　work　provides　a　green　and　sustainable　strategy　for　the　production　of　secondary　amines　using　alcohols　as　the　alkylating　agent.　This　study　also　demonstrates　the　unique　advantages　of　2D　MOF　ultrathin　nanosheets　in　the　fabrication　of　multifunctional　catalytic　systems　for　light　initiated　one-pot　tandem/cascade　reactions.