In　this　work,　a　simple,　low-cost,　green,　and　mild　method　for　the　preparation　of　three-dimensional　nanocomposite　materials　of　gold　nanorods　(Au　NRs)@TiO2　is　reported.　The　surface　of　Au　NRs　was　coated　with　TiO2　in　situ　reduction　at　room　temperature　without　a　complicated　operation.　The　synthetic　Au　NRs@TiO2　nanocomposites　were　used　as　surface-enhanced　Raman　spectroscopy　(SERS)　active　substrates　for　the　reusable　and　sensitive　detection　of　environmental　pollutants.　The　results　showed　that　the　pollutants　on　Au　NRs@TiO2　nanocomposites　have　higher　SERS　activity　and　reproducibility　than　those　on　the　Au　NR　substrate　without　the　presence　of　TiO2.　Moreover,　the　SERS　substrate　can　be　readily　recycled　by　UV-assisted　self-cleaning　to　remove　residual　analyte　molecules.　Malachite　green　(MG)　and　crystal　violet　(CV)　were　used　as　examples　to　demonstrate　the　feasibility　of　the　proposed　sensor　for　the　sensitive　detection　of　environmental　pollutants.　The　results　showed　that　the　limit　of　detections　(LODs)　were　0.75　μg/L　and　0.50　μg/L　for　MG　and　CV,　respectively,　with　the　recoveries　ranging　from　86.67%　to　91.20%　and　83.70%　to　89.00%.　Meanwhile,　the　SERS　substrate　can　be　easily　regenerated　by　UV　light　irradiation.　Our　investigation　revealed　that　within　three　cycles,　the　Au　NRs@TiO2　substrates　still　maintained　the　high　SERS　enhancement　effect　that　they　showed　when　first　used　for　SERS　detection.　These　results　indicated　that　the　method　can　be　used　to　detect　MG　and　CV　in　really　complex　samples.　Due　to　the　high　sensitivity,　reusability,　and　portability　and　the　rapid　detection　property　of　the　proposed　sensor,　it　can　have　potential　applications　in　the　on-site　detection　of　environmental　pollutants　in　a　complex　sample　matrix.　©　2022　by　the　authors.