Evidence of the association between 25-hydroxyvitamin D (25(OH)D) and metabolic syndrome (MeS) remains uncertain and incongruent. This study aimed to determine the association between 25(OH)D and MeS among Jordanian adults. A complex multistage sampling technique was used to select a national population-based household sample. The present report deals exclusively with adults aged > 18 years who had complete information on all components of MeS (n = 3,234). A structured questionnaire was used to collect all relevant information. Anthropometric, clinical, and laboratory measurements were obtained. MeS was defined according to the International Diabetes Federation (IDF) definition. Of the total, 42.0% had MeS and 31.7% had 25(OH)D < 30 ng/ml. In a stratified analysis, the prevalence of MeS did not differ significantly between subjects with low and normal 25(OH)D levels for men and women in all age groups. In the multivariate analysis, the odds of MeS were not significantly different between subjects with low and normal 25(OH)D levels (OR = 0.85, 95% CI: 0.70, 1.05, P-value = 0.133). The association between 25(OH)D and MeS remained non-significant when 25(OH)D was analyzed as a continuous variable (OR = 1.004, 95% CI; 1.000, 1.008, P = 0.057) and when analyzed based on quartiles. None of the individual components of MeS were significantly associated with 25(OH)D level. This study does not provide evidence to support the association between 25(OH)D level and MeS or its individual components. Prospective studies are necessary to better determine the roles of 25(OH)D levels in the etiology of MeS.