As the relationship between vitamin D and various diseases or health conditions has become known, interest in the contribution of vitamin D to overall health-related quality of life (QoL) has increased. We examined the relationship between vitamin D status and QoL in 273 participants aged 65 years and older. Serum levels of total calcium, phosphorus, intact parathyroid hormone, albumin, and 25-hydroxyvitaminD3 were analyzed. We also recruited data for QoL, physical activity, nutritional impairment, and muscular strength. Ninety percent of the subjects were classified as vitamin D deficient or insufficient. Participants with higher serum 25(OH)D3, calcium, phosphorous, and Alb levels were significantly less likely to self-report depression or anxiety after adjustment (p = 0.009, p = 0.005, p = 0.003, and p = 0.005, respectively). Additionally, we found an association between lower levels of albumin and self-reported problems with mobility or usual activities (p = 0.01). We also found associations between better muscle strength and higher levels of vitamin D, calcium, phosphorous, and albumin (p = 0.006, p = 0.003, p = 0.004 and p = 0.002, respectively). Overall, our data provide evidence that serum vitamin D and Alb levels are negatively related to self-reported anxiety or depression, usual activities, mobility, and three dimensions of QoL in older adults. Furthermore, vitamin D levels are positively related to hand grip strength in adults over 65 years old.