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Microgreens have recently gained popularity owing to their reliable economic and nutritional value. This study aimed to increase the quality of microgreen broccoli via treatment with different concentrations (1%, IPB-1; 3%, IPB-3; 5%, IPB-5; or 7%, IPB-7 w/v) of illite—a natural mineral powder. The results showed that the illite treatments considerably increased the content of mineral elements, such as Ca, P, and K; of vitamin C; and of free amino acids; and also increased the total weight of the broccoli sprouts. The content of sulforaphane, a bioactive compound, also increased by up to 47% with illite treatment, with the highest increase being in the IPB-5 group. However, several of the parameters were lower in the IPB-7 group. Aromatic compounds were categorized by functional groups such as hydrocarbons which numbered 36, 30, 34, 28, and 30 in the control, IPB-1, IPB-3, IPB-5, and IPB-7 groups, respectively. We found 16, 15, 15, 13, and 14 sulfides, including dimethyl sulfide, in the control, IPB-1, IPB-3, IPB-5, and IPB-7 groups, respectively. Additionally, aldehydes, comprising seven compounds, were detected in the IPB-1, IPB-3, IPB-5, and IPB-7 groups. Illite treatment significantly increased the activities of antioxidants such as DPPH and the polyphenol content of the microgreens. These results indicate a potential role for appropriate illite doses in microgreen treatment to address multinutrient deficiencies and to increase the quality of microgreen vegetables. [ABSTRACT FROM AUTHOR]