As an important crop in the world, dried pepper is widely used in various foods. However, the sensory quality, fruit shape index, edible index, nutrition index, and volatile components of dried pepper have not been comprehensively analyzed. This study elucidated the differences between different varieties of dried pepper and provided the basis for the selection of raw materials for different varieties of dried pepper products. The varieties with high scores in sensory evaluation were Henan new generation, Neihuang new generation, Chengdu Erjingtiao, India S17, and Honglong 12. The varieties with the highest fruit shape index, edible rate, and nutrition index were Chengdu Erjingtiao and Guizhou Erjingtiao. A total of 380 volatile organic compounds were identified by comprehensive two-dimensional gas chromatography-time-of-flight mass spectrometry with headspace sampling (HS-GC-TOF MS), including 62 alcohols, 50 aldehydes, 68 ketones, 60 hydrocarbons, 99 esters, 18 acids, and 23 other substances such as pyrazoles and ethers.