Background: Jaundice, characterized by elevated serum bilirubin levels, reflects underlying hepatic dysfunction, which may impair vitamin D metabolism. Vitamin D deficiency is increasingly recognized as a frequent complication in liver disorders, but its prevalence and association with jaundice are not well established. Aim of the Study: The present investigation aimed to assess the frequency of vitamin D deficiency among individuals diagnosed with jaundice and to explore the correlation between vitamin D status and serum bilirubin concentrations. Methodology: The study enrolled 150 patients with jaundice confirmed through clinical and biochemical assessments, alongside 50 healthy control subjects. Serum levels of 25-hydroxyvitamin D [25(OH)D] and total bilirubin were quantitatively measured and analyzed. Serum-vitamin D ranks were stratified into three-groups: deficiency (<20 ng/mL), insufficiency (20–29 ng/mL), and sufficiency (≥30 ng/mL). Results: Vitamin D-deficiency was significantly more predominant among jaundiced patients compared to controls (72% vs. 38%, p < 0.001). Patients with insufficient vitamin D were identified in 18% of patients and 34% of controls, while only 10% of patients had sufficient levels compared to 28% of controls. An inverse and statistically significant relationship was identified between serum bilirubin and vitamin D levels (r = -0.42, p < 0.001), showing that greater bilirubin levels were linked with lower serum vitamin D concentrations. Conclusions: Vitamin D-deficiency is extremely predominant in jaundiced patients and correlates inversely with the severity of hyperbilirubinemia. Regular assessment of vitamin D-status in jaundiced people could support timely therapeutic strategies and enhance overall patient prognosis.