Chinese water chestnut (CWC) is popular among consumers due to its unique flavor and crisp and sweet taste. Thus far, the key substances affecting the taste compound of CWC are still unclear. In this study, we used UPLC-MS/MS and an electronic tongue system to study the effects of four typical steaming and cooking methods, cooking without peel for 10 min (PC), steaming without peel for 15 min (PS), cooking with peel for 30 min (WPC), steaming with peel for 30 min (WPS), on the taste compound generation and variation of CWC, and revealed the secret of its crisp and sweet taste. The results show that the electronic tongue can effectively identify the taste profile of CWC, and the effective tastes of CWC were umami, bitterness, saltiness, and sweetness. We screened 371 differential compounds from 640 metabolic species. Among them, nucleotides and their derivatives, carbohydrates, organic acids and their derivatives, and amino acids and their derivatives are closely related to the key taste of CWC, and these compounds affected the taste of CWC through six related metabolic pathways: oxidative phosphorylation and purine metabolism; alanine, aspartate, and glutamate; bile secretion; amino sugar and nucleotide sugar metabolism; the phenylpropane pathway; and toluene degradation. This study reveals the potential metabolic causes of taste compound generation and variation in the taste of CWC.