Primary liver cancer is one of the most common malignant tumors worldwide, and the incidence and mortality rates in many Western countries are on the rise. Only a small percentage of liver cancer patients are suitable for curative therapy such as surgical resection and liver transplantation, leaving the majority of patients with palliative options. However, advanced liver cancer is generally resistant to the currently available treatments such as chemotherapy and radiotherapy. Thus, the conventional treatments only have limited effects for patients with liver cancer. Considering the unique dual blood supply system of the liver, and the important role of angiogenesis in the development of primary liver cancer, combination of transarterial embolization (TAE) or transarterial chemoembolization (TACE) with molecular drugs targeting angiogenesis may hold a great therapeutic potential.