Mica is a kind of important rock-forming mineral in the lithosphere of Earth, which can be a superior tool used to trace the origin and late evolution of rock. The Jian forsterite jade (a kind of geological skarn) is an emerging kind of gemstone in China with a beautiful color and luster, discovered in Ji’an County, Jilin Province, Northeast China. It is mainly composed of rare Mg-rich forsterite (Mg# (Mg/(Mg+Fe2+) up to 99), serpentine and brucite. The source of hydrothermal fluid triggering the late metamorphism (the serpentinization of forsterite) of forsterite jade deposits remains unclear. We report a series of phlogopites with a regular range of mineral compositions in the forsterite jade deposit. Micrographs show that the phlogopites are associated with forsterite and coexist with serpentine in forsterite jade, tourmaline and tremolite in the contact zone, and plagioclase in pegmatite, and the related replacement of phlogopite seems to have not occurred. The phlogopites that occurred as single grains or veinlets in forsterite jade named type I are characterized by high XMg, ranging from ~0.98 to ~0.95, and the phlogopites that occurred in the contact zone of forsterite jade and pegmatite named type II are rich in Fe, with a range of XMg from ~0.82 to ~0.66. Additionally, the type II phlogopites are also rich in Ti, Mn, Cl, Li, Rb, Zn, V, Co, Nb and Ta but poor in Na, Sr and F compared to the type I phlogopite. Petrological and mineralogical characteristics and geochemical compositions suggest that the phlogopites are crystallized from the corresponding fluid component by hydrothermal metasomatism. The abundant Mg of the fluid phase is produced during the serpentinization of forsterite, triggered by pegmatitic hydrothermal fluid, and other main materials like K, Al, Si and H2O are provided by the intrusive pegmatite. With the occurrence of and regular compositional variation in phlogopites in the forsterite jade deposit, we suppose that the hydrothermal fluid triggering the serpentinization of the Jian forsterite jade is produced by the intrusive pegmatite.