The　multicomponent　composite　nanomaterials　with　multilevel　spatial　structures　have　a　broad　application　prospect　in　energy　conversion.　Herein,　we　rationally　designed　a　novel　strategy　to　synthesize　hierarchical　yolk-shelled　N-doped　carbon/CoS2/MoS2　nano　polyhedrons　(NC-CoS2@CoS2/MoS2　YSPs)　as　bifunctional　catalysts　for　dye-sensitized　solar　cells　(DSSCs)　and　hydrogen　evolution　reactions　(HERs).　NC-CoS2@CoS2/MoS2　YSPs　were　prepared　by　ion-exchange　between　zeolitic　imidazolate　framework-67　(ZIF-67)　and　(NH4)2MoS4　with　a　subsequent　sulfuration　reaction　under　an　annealing　treatment.　Benefiting　from　the　unique　yolk-shelled　architecture,　the　obtained　NC-CoS2@CoS2/MoS2　YSPs　had　enough　internal　clearance　for　both　accommodating　electrolyte　and　loading　abundant　active　sites.　In　addition,　the　introduction　of　N　and　C　elements　greatly　improved　the　activity　and　electroconductibility　of　the　catalysts.　As　a　result,　the　DSSC　based　on　NC-CoS2@CoS2/MoS2　YSPs　exhibited　a　superior　power　conversion　efficiency　of　9.54%,　which　was　apparently　higher　than　that　of　Pt　(8.19%).　Furthermore,　a　low　onset　potential　of　44.5　mV　and　a　small　Tafel　slope　of　64.6　mV　dec–1　were　achieved　by　this　catalyst　for　HER　in　0.5　M　H2SO4.　The　present　approach　affords　a　new　idea　for　the　design　of　yolk-shelled　nanomaterials　and　can　be　extended　to　synthesize　other　catalysts　to　substitute　Pt-based　materials　in　different　energy　conversion　fields.　©　2020　Elsevier　B.V.