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As technology continues to advance, the development of novel sensing systems opens new possibilities for low-cost, practical biosensing applications. In this Letter, we demonstrate a localized surface plasmon resonance system that combines both wave-guiding and plasmonic resonance sensing with a single microstructured polymeric structure. Characterizing the sensor using the finite element method simulation shows, to the best of our knowledge, a record wavelength sensitivity (WS) of 111000 nm/refractive index unit (RIU), high amplitude sensitivity (AS) of 2050  RIU^−1, high sensor resolution and limit of detection of 9×10^−7 RIU and 8.12×10^−12  RIU^2/nm, respectively. Furthermore, these sensors have the capability to detect an analyte within the refractive index range of 1.33–1.43 in the visible to mid-IR, therefore being potentially suitable for applications in biomolecular and chemical analyte detection.