Angiogenesis, the development of new blood vessels, is an important pathological component of diseases such as cancer and heart disease. Since the genomics-focused drug-discovery efforts to produce the expected large number of compounds have encountered many difficulties, the attempts to find active ingredients with angiogenesis modulating properties from plants or herbs have entered our visual field in recent years. Particularly, some traditional Chinese herbs have a long and successful history for the treatment of angiogenesis-related diseases, which offered a safer and more effective angiotherapy approach. The dried root and rhizome of Salvia miltiorrhiza (also known as Danshen in China), one of the most important traditional Chinese herbs, is commonly used in clinics for the treatment of cardiovascular and cerebrovascular diseases. Although a few of efforts have been maid to explore the angiogenic properties of S. miltiorrhiza, there still remains lots of works to be developed to correlate the chemical components with the pharmacological properties of this precious Chinese herb. Therefore, in this present study, a systematic research on the chemical constituents, pharmacological characteristics and quantity control of S. miltiorrhiza focusing on the antiangiogenic activity was carried out. The major achievements are summarized as follows: (1) 13 diterpenoid compounds of S. miltiorrhiza were obtained from the chloroform extract of hydrophobic fraction using sequential silica-gel-column chromatographic separation and repeated re-crystallization. This provides the screened samples for pharmacological study and the markers for quality control. (2) The antiangiogenic properties of the diterpenoid compounds in S. miltiorrhiza were explored using in vitro assays. Some of these diterpenoid compounds showed antiangiogenic activities via multiple mechanisms, including the inhibitory effects on the proliferation, invasion and tube formation of HUVECs. (3) The structure-activity relationships (SAR) of the tested compounds as angiogenesis inhibitors were discussed for the first time. According to the prediction of SAR, 15,16-dihydrotanshinone I should have the most predominant inhibitory effect on VEGF-induced angiogenesis, which is consistent with the findings in the current study. (4) Western blot analysis was applied to reveal the underlying mechanism, which indicated that the antiangiogenic effects of these diterpenoid compounds in S. miltiorrhiza, were partially through the blockade of the ERK and PI3K signaling pathway. (5) Pressurized liquid extraction (PLE) coupled with capillary electrochromatography (CEC), high performance liquid chromatography (HPLC) and ultra performance liquid chromatography (UPLC) were developed to assay the major diterpenoid compounds in S. miltiorrhiza for the first time. These analytical methods have been validated as rapid, sensitive, accurate and reproducible strategies for quality evaluation of S. miltiorrhiza. In summary, the present study systematically explored the antiangiogenic activites and the novel techniques for the quality control of S. miltiorrhiza. Some potential antiangiogenic compounds, such as 15,16-dihydrotanshinone I and miltirone, were identified for the first time. Furthermore, several efficient, sensitive and reliable methods for the quality evaluation of S. miltiorrhiza were developed. These works will help to elucidate the main active components, deepen the understanding of the pharmacological effects and accurately control the quality of the herbal material and related products.