Wall rocket is a wild vegetable with interest to become a crop. However, the information regarding morphological variability in the species is scarce, despite the interest it has received for breeding programs. In addition, evaluating the phytochemical composition can also be useful for developing materials of a high quality. In this study, forty-four populations were evaluated for selected morphoagronomic traits and contents in ascorbic acid (AA), total phenolics (TP), and nitrates (NO3−). Wall rocket plants had, on average, an intermediate growth habit and a good response to transplant. Moderate variability, mainly for size-related traits, was found, with low to moderate heritability estimates (H2 < 0.35). A Principal Component Analysis revealed that some materials may be selected for differenced traits. On the other hand, wall rocket materials had, on average, high contents in AA (53 mg 100 g−1) and TP (116 mg CAE 100 g−1) but also accumulated high levels of NO3− (891 mg 100 g−1). Significant positive correlations were found for AA and TP, which could be exploited for increasing the antioxidant activity and properties of the final product. We provide new information on the variation of wall rocket for traits of morphological and phytochemical interest, which together with other traits, such as the profile of glucosinolates, can be useful for the selection of materials in future breeding programs.