Various epidemiological studies have demonstrated that vitamin D may play important roles in the pathogenesis and progression of cancer. Vitamin D is one of the most pivotal nutraceuticals whose active metabolite, calcitriol (1,25-dihydroxyvitamin D3), possesses anti-proliferative, pro-apoptotic, and pro-differentiating capabilities. Accumulating evidence indicates that the potential benefits of using vitamin D in cancer are not only anti-cancer cell proliferation which is linked with its anti-inflammatory effects, including the suppression of prostaglandin metabolism and inhibition of NF-κB signaling, but also suppressing tumor metastasis and angiogenesis. Here, we present a systematic summary of the effects of vitamin D in the chemoprevention and chemotherapy of cancer, especially anti-metastatic and anti-angiogenic actions.