In light of the growing body of literature suggesting a beneficial effect of vitamin D on inflammatory response, we hypothesized that vitamin D affects serum ferritin (SF), a biomarker of inflammation. The objective of the present study is to examine the association of serum 25-hydroxyvitamin D [25(OH)D] with elevated SF concentrations indicative of inflammation as no earlier study has done so. Data from 5550 Canadian adults who participated in the 2012/2013 and the 2014/2015 Canadian Health Measures Surveys were analysed. We observed that 9.4% of Canadian adults have elevated SF concentrations and that 35.6% were vitamin D insufficient. Among Canadians with under/normal body weights, those with serum 25(OH)D ≥ 75 nmol/L relative to those with serum 25(OH)D < 50 nmol/L, were substantially less at risk for elevated SF concentrations (OR = 0.24; 95% CI = 0.06, 0.89; p = 0.034). We did not observe this association for overweight and obese Canadians. Canadians of older age, non-white ethnicity, males, those with income above $100,000, those who consumed alcohol, and those with high total cholesterol concentrations and elevated blood pressures were more likely to have elevated SF concentrations. Serum 25(OH)D ≥ 75 nmol/L is likely to provoke anti-inflammatory benefits, but intervention studies that achieve high 25(OH)D concentrations and with long follow up are needed to establish the role of vitamin D on SF.