Asian populations habitually consume a large amount of cruciferous vegetables and other plant-based foods. Few epidemiologic investigations have evaluated the potential health effects of these foods in Asian populations. We aimed to examine the associations of cruciferous vegetables, noncruciferous vegetables, total vegetables, and total fruit intake with risk of all-cause and cause-specific mortality. The analysis included 134,796 Chinese adults who participated in 2 population-based, prospective cohort studies: the Shanghai Women's Health Study and the Shanghai Men's Health Study. Dietary intakes were assessed at baseline through in-person interviews by using validated food-frequency questionnaires. Deaths were ascertained by biennial home visits and linkage with vital statistics registries. We identified 3442 deaths among women during a mean follow-up of 10.2 y and 1951 deaths among men during a mean follow-up of 4.6 y. Overall, fruit and vegetable intake was inversely associated with risk of total mortality in both women and men, and a dose-response pattern was particularly evident for cruciferous vegetable intake. The pooled multivariate hazard ratios (95% CIs) for total mortality across increasing quintiles of intake were 1 (reference), 0.91 (0.84, 0.98), 0.88 (0.77, 1.00), 0.85 (0.76, 0.96), and 0.78 (0.71, 0.85) for cruciferous vegetables (P < 0.0001 for trend) and 0.88 (0.79, 0.97), 0.88 (0.79, 0.98), 0.76 (0.62, 0.92), and 0.84 (0.69, 1.00) for total vegetables (P = 0.03 for trend). The inverse associations were primarily related to cardiovascular disease mortality but not to cancer mortality. Our findings support recommendations to increase consumption of vegetables, particularly cruciferous vegetables, and fruit to promote cardiovascular health and overall longevity.