A multifunctional Au-coated TiO2 nanotube array is made via synthesis of a TiO2 nanotube array through a ZnO template, followed by deposition of Au particles onto the TiO2 surface using photocatalytic deposition and a hydrothermal method, respectively. Such arrays exhibit superior detection sensitivity with high reproducibility and stability. In addition, due to possessing stable catalytic properties, the arrays can clean themselves by photocatalytic degradation of target molecules adsorbed to the substrate under irradiation with UV light into inorganic small molecules using surface-enhanced Raman spectroscopy (SERS) detection, so that recycling can be achieved. Finally, by detection of Rhodamine 6G (R6G) dye, herbicide 4-chlorophenol (4-CP), persistent organic pollutant (POP) dichlorophenoxyacetic acid (2,4-D), and organophosphate pesticide methyl-parathion (MP), the unique recyclable properties indicate a new route in eliminating the single-use problem of traditional SERS substrates and show promising applications for detecting other organic pollutants.