Self-assembled　structures　of　2D　materials　with　novel　physical　and　chemical　properties,　such　as　the　good　electrical　and　optoelectrical　performance　in　nanoscrolls,　have　attracted　a　lot　of　attention.　However,　high　photoresponse　speed　as　well　as　high　responsivity　cannot　be　achieved　simultaneously　in　the　nanoscrolls.　Here,　a　photodiode　consisting　of　single　MoS2　nanoscrolls　and　a　p-type　WSe2　is　demonstrated　and　shows　excellent　photovoltaic　characteristics　with　a　large　open-circuit　voltage　of　0.18　V　and　high　current　intensity.　Benefiting　from　the　heterostructure,　the　dark　current　is　suppressed　resulting　in　an　increased　ratio　of　photocurrent　to　dark　current　(two　orders　of　magnitude　higher　than　the　single　MoS2　nanoscroll　device).　Furthermore,　it　yields　high　responsivity　of　0.3　A　W-1　(corresponding　high　external　quantum　efficiency　of　approximate　to　75%)　and　fast　response　time　of　5　ms,　simultaneously.　The　response　speed　is　increased　by　three　orders　of　magnitude　over　the　single　MoS2　nanoscroll　device.　In　addition,　broadband　photoresponse　up　to　near-infrared　could　be　achieved.　This　atomically　thin　WSe2/MoS2　nanoscroll　integration　not　only　overcomes　the　disadvantage　of　MoS2　nanoscrolls,　but　also　demonstrates　a　single　nanoscroll-based　heterostructure　with　high　performance,　promising　its　potential　in　the　future　optoelectronic　applications.