Spontaneously dried-fermented radishes have been consumed in China for hundreds of years and are usually fermented for a long time to acquire high quality. In this study, the spontaneously dried-fermented radishes with short-term manufacturing periods were made from five different varieties of radishes that grew in the same environment. In addition, the physicochemical characteristics (i.e., moisture content, soluble solid, and pH value), flavor profiles (i.e., free amino acids, organic acids, and volatile compounds), and functional properties (i.e., total phenolics content, total flavonoids content, sulforaphane content, and γ-aminobutyric acid [GABA] content) of these five raw radishes and spontaneously dried-fermented radishes were analyzed and compared. In detail, the content of volatile and nonvolatile compounds increased, especially in oxalic acid, succinic acid, and umami free amino acids. Furthermore, functional components, such as sulforaphane and GABA, were also enriched via spontaneous fermentation after drying. In addition, the results of principal component analysis, hierarchical clustering analysis, and redundancy analysis showed that there were significant discrepancies appeared when raw radishes were processed via spontaneous fermentation or not. These results suggested that the process of spontaneous fermentation after drying may contribute to improving the quality of fresh radishes. Notably, radishes with red skin and flesh were regarded as exceptional varieties for processing, because of the preferable flavor profiles and affluent functional substances via spontaneous fermentation after drying. Therefore, these findings could deliver a systematical insight into developing processed radishes with high quality. PRACTICAL APPLICATION: The spontaneously dried-fermented radishes were manufactured through the process of spontaneous fermentation after drying, which acquired tasty and healthy characteristics by accumulating the volatile and nonvolatile compounds as well as the functional components, like total phenolics, total flavonoids, sulforaphane, and γ-aminobutyric acid. Importantly, because of the excellent processing properties, the radishes with red skin and flesh could be more appropriate to produce spontaneously dried-fermented radishes. Our findings may provide a practical strategy for developing vegetable relishes with superb flavor profiles and good functional properties in pickled vegetables.