Headspace-gas chromatography-ion mobility spectrometry (HS-GC-IMS) was used to analyze the volatile substances of dried Capsicum frutescens with 4 different drying methods in this study, including hot air drying, infrared drying, vacuum freeze drying, and sun drying. The results showed that 39 volatile substances were identified, including 9 esters, 10 aldehydes, 10 alcohols, 2 furans, 3 pyrazines, 3 ketones, and 2 organic acids. Esters, aldehydes, and alcohols were the main volatile substances of dried Capsicum frutescens. Principal component analysis (PCA) and heat map clustering results showed that the volatile substances of samples treated by hot air drying had high relevance with the ones with infrared drying compared to vacuum freeze drying and sun drying. Compared with hot air drying and infrared drying, vacuum freeze drying and sun drying exhibited different effects on the volatiles flavor substances of Capsicum frutescens. Some volatile substances had obvious correlation during the drying process, such as esters and alcohols, alcohols and aldehydes, and they could realize the conversion of volatile flavor compounds through chemical reactions. Drying methods had little influence on volatile substances. There were 39, 37, 36, and 34 volatile substances in hot air drying, infrared drying, vacuum freeze drying and sun drying of Capsicum frutescens, respectively. However, drying method had obvious influence on volatile substances content of Capsicum frutescens. Esters, furans, and pyrazines in samples treated by hot air drying and infrared drying had higher content than vacuum freeze drying and sun drying, while the samples treated by vacuum freeze drying and sun drying had higher content in aldehydes than hot air drying and infrared drying ones. Overall, hot air drying and infrared drying had positive effects on enriching the flavor of dried Capsicum frutescens. This study will provide a theoretical basis for the processing and flavor quality control of dried Capsicum frutescens.