Carbon-supported　metal　nanoparticles　(NPs)　play　important　roles　in　heterogeneous　catalysis.　In　particular,　supported　bimetallic　catalytic　systems　can　be　promising　multifunctional　catalysts　for　one-pot　tandem/cascade　reactions,　in　which　two　or　more　successive　independent　reactions　are　realized　in　one　pot.　In　this　manuscript,　we　report　the　preparation　of　a　carbon-supported　bimetallic　CoCu　catalytic　system　(Co−C@Cu−C),　with　Co　NPs　wrapped　by　carbon-supported　Cu　NPs,　from　the　pyrolysis　of　a　core-shell　structured　Co−MOF-74@Cu−MOF-74.　The　as-obtained　Co−C@Cu−C　acts　as　a　bifunctional　catalyst　for　the　transformation　of　phenylacetylene　to　1,　4-diphenyl-1,　3-butadiene　in　one　pot,　in　which　supported　metallic　Cu　NPs　and　Co　NPs　are　active　for　the　coupling　and　hydrogenation　reaction　respectively.　By　tuning　the　reaction　rates　of　the　coupling　and　the　hydrogenation　in　this　tandem　reaction　over　the　Co−C@Cu−C　via　changing　the　reaction　medium　and　the　reducing　agent,　an　efficient　direct　transformation　of　phenylacetylene　to　1,　4-diphenyl-1,　3-butadiene　was　realized.　This　work　not　only　highlights　the　important　role　of　MOFs　in　the　preparation　of　multifunctional　carbon　supported　metal　NPs　for　heterogeneous　catalysis,　but　also　demonstrates　the　possibility　of　tuning　the　reaction　rates　of　different　catalytic　steps　in　a　tandem　reaction　to　realize　an　efficient　overall　reaction.　©　2020　Wiley-VCH　GmbH