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Purpose: The relationship between vitamin D levels and cancer incidence and mortality in individuals with metabolic syndrome (MetS) remains poorly explored. Herein, we aimed to determine the association between 25-hydroxyvitamin D [25(OH)D] concentrations and the risk of 16 cancer incidence types and cancer/all-cause mortality in patients with MetS. Methods: We enrolled 97,621 participants with MetS at recruitment from the UK Biobank cohort. The exposure factor was baseline serum 25(OH)D concentrations. The associations were examined using Cox proportional hazards models, which were displayed as hazard ratios (HRs) with 95% confidence intervals (CIs). Results: Over a median follow-up period of 10.92 years for cancer incidence outcomes, 12,137 new cancer cases were recorded. We observed that 25(OH)D concentrations were inversely related to the risk of colon, lung, and kidney cancer, and HRs (95% CI) for 25(OH)D ≥ 75.0 vs. < 25.0 nmol/L were 0.67 (0.45–0.98), 0.64 (0.45–0.91), and 0.54 (0.31–0.95), respectively. The fully adjusted model revealed a null correlation between 25(OH)D and the incidence of stomach, rectum, liver, pancreas, breast, ovary, bladder, brain, multiple myeloma, leukemia, non-Hodgkin lymphoma, esophagus, and corpus uteri cancer. Over a median follow-up period of 12.72 years for mortality outcomes, 8286 fatalities (including 3210 cancer mortalities) were documented. An "L-shaped" nonlinear dose–response correlation was detected between 25(OH)D and cancer/all-cause mortality; the respective HRs (95% CI) were 0.75 (0.64–0.89) and 0.65 (0.58–0.72). Conclusion: These findings emphasize the importance of 25(OH)D in cancer prevention and longevity promotion among patients with MetS. [ABSTRACT FROM AUTHOR]