Abstract: A gas chromatography-mass spectrometry (GC-MS) method was developed for the simultaneous determination of quinoline, pyridine, and crotonaldehyde in footwear materials. Using methanol as the extraction solvent and ultrasonic-assisted extraction, key parameters were systematically optimized, including extraction solvent type, temperature, time, solvent volume, chromatographic column, injector temperature, heating rate, and carrier gas flow rate. The test results show that within the curve range of 0.05–1.0 mg/kg, the average recoveries of the target compounds are 90.22%–110.89% and the relative standard deviations are 0.79%–6.76%, indicating good precision. The detection results are accurate and reliable, which can meet the requirements of qualitative and quantitative detection. This method provides a technical reference for the risk monitoring of footwear products and protects human health and environmental safety.