The　ability　to　reproducibly　create　a　surface　enhanced　Raman　scattering　(SERS)　substrate　renders　an　effective　means　of　detecting　and　degrading　organic　contaminants.　Vertically　aligned　(VA)　nanomaterials　have　been　extensively　explored　as　highly　efficient　catalysts　due　to　their　excellent　electron　transportability　and　high　concentration　of　exposed　active　edge　sites.　Herein,　we　report　on　a　ternary　ultrafast-electron-transfer　heterostructure　composed　of　Pt　nanoparticles　in-situ　grown　on　VA-MoS2　nanosheet　edge　sites　decorated　on　TiO2　nanotube　arrays　(NTAs)　(denoted　Pt/VA-MoS2/NTAs).　Compared　with　pristine　TiO2　NTAs,　the　Pt/VA-MoS2/NTAs　possess　a　strong　resonant　SERS　effect　for　detecting　rhodamine　6G　and　an　outstanding　UV-assisted　self-cleaning　effect,　displaying　an　excellent　photocatalytic　performance　under　visible　light　irradiation.　Such　markedly　improved　performance　of　the　ternary　Pt/VA-MoS2/TiO2　NTAs　nanocomposites　can　be　attributed　to　the　synergy　of　catalytic　activity　of　Pt-deposited　MoS2　edge　sites,　the　ultrafast　electron　transfers　of　VA-MoS2　NS/TiO2　NTAs,　and　the　appropriate　band　alignment　among　these　three　constituents.　As　such,　it　represents　a　robust　mean　of　developing　advanced　energy　utilization　nanocomposites　for　high-performance　catalysts　and　sensors.