Hornblende is one of the widely distributed rock-forming minerals, and the contents of Mg²⁺ and Fe²⁺ are the basis for naming tremolite-ferroactinolite series, which is of great significance to the research of mineralogy, petrology and gemmology. In this paper, tremolite-ferroactinolite series samples from eight places of different origin were collected, and systematic Raman spectroscopy and electron probe quantitative analysis were carried out. It was found that the Raman spectrum peaks of hornblende series minerals varied regularly in the range of 3 600～3 700 cm^-1, and the peak area had a good linear correlation with the contents of magnesium and iron obtained by electron probe. The method of calculating Mg²⁺ and Fe²⁺ contents in tremolite-ferroactinolite by Raman peak area is concluded, which can be applied to rapid and non-destructive analysis for tremolite-ferroactinolite series minerals.