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In this work, multimodal responsive optical waveguide sensors using a stable cross-linking gel polymer electrolyte are successfully designed and fabricated by bottom metal-printing technology. Temperature and humidity sensing characterization based on the polymer electrolyte is simulated and analyzed. The multimodal responsive properties of the photonic chip are defined based on the analysis of ion relaxation dynamics: optical phase variable to monitor temperature and optical attenuation variable to detect humidity. In the supervising temperature (36.0-38.0 °C) and relative humidity (45-65%) range, the temperature and humidity sensitivities of the device are measured as 0.5π rad/°C and 1.14 dB/% RH, respectively. The fast-response time for both temperature and humidity of the multifunctional sensor can be obtained as 4.21 ms and 1.32 s, respectively. These findings provide a feasible scheme for the design and application of temperature and humidity sensors in potential medical treatment. From gel polymer electrolytes to multimode monitoring applications, the application exploration of high stability and ultrafast response multimode waveguide sensors is gradually being carried out. This study has great significance for the comprehensive monitoring of sophisticated human physical signs by multimodal responsive waveguide sensors.