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Microstructure fibers, integrating microfluidic channels and light guidance in one fiber, enable three-dimensional surface-enhanced Raman scattering (SERS) detection for large signal accumulation. However, the available fiber SERS probes are complicated to prepare and they are not reusable. In addition, light interacts with analytes in a form of an evanescent field, which is very weak. In this paper, we developed a SERS platform based on suspended-core photonic crystal fibers decorated with Ag/ZnO nanocomposites on the inner surface for direct, ultrasensitive, and reusable analyte detection. The unique configuration not only transfers a core-localized field to the liquid interface to greatly enhance the light–analyte interaction but also facilitates charge transfer to further improve the SERS detection sensitivity and degradation efficiency. The detection limit of crystal violet solution is 10–13 M, and the enhancement factor reaches 1011. The relative standard deviation is as low as 5.4%, ensuring the reproducibility of SERS detection. The probe has good photocatalytic performance and can degrade molecules under ultraviolet-light illumination within 20 min. This ultrasensitive and reusable SERS probe shows great application potential in rapid and in situ liquid detection. [ABSTRACT FROM AUTHOR]