Abstract: Anisi Stellati Fructus is the fruit of Illicium verum Hook. F. (Chinese star anise), which is a significant Chinese medicinal herb. It is reported to possess antimicrobial, antiviral, and antioxidant properties, and has also been documented to improve digestion and alleviate symptoms of dysentery, dyspepsia, asthma, flatulence, menstrual irregularities, colic, inflammation, bronchitis, and rheumatic diseases. At present, a variety of compounds have been isolated from Anisi Stellati Fructus. This study systematically investigated the chemical components of Anisi Stellati Fructus by a method of ultra-high-performance liquid chromatography-quadrupole Orbitrap high-resolution mass spectrometry (UPLC-Q-Orbitrap-HRMS) combined with comprehensive two-dimensional gas chromatography-mass spectrometry (GC×GC-MS). For the non-volatile constituents, the methanol extract of Anisi Stellati Fructus was separated prior to MS analysis using a Waters BEH C18 column (100 mm×2.1 mm, 1.7 μm) with a gradient elution system consisting of 0.1% formic acid aqueous solution and acetonitrile as the mobile phase. Mass spectrometric detection was performed under both positive and negative electrospray ionization (ESI) modes, and the major chromatographic peaks were identified based on accurate mass measurements, secondary mass spectral fragmentation patterns, consulting literature reports, mass spectrometry databases, fragmentation regularities of mass spectra, retention time, as well as reference compounds. For the volatile components, headspace solid-phase microextraction (HS-SPME) was employed for sample introduction. The separation was achieved using a combination of DB-Heavywax (30 m×250 μm, 0.25 μm) and DB-17 MS (1.1 m×180 μm, 0.18 μm) capillary columns under temperature programming. Electron ionization (EI) was used for ionization, with a mass scanning range of m/z 45-550. The identification of volatile compounds was accomplished by combining NIST standard spectral library searches with information from published literatures. The results showed that UPLC-Q-Orbitrap-HRMS identifies 45 compounds, including 13 phenylpropanoids, 8 phenolic acids, 18 flavonoids, and 6 other compounds. Meanwhile, GC×GC-MS identifies 108 volatile components, which are categorized into 66 terpenoids, 8 phenylpropanoids, 7 alkanes, 10 esters, 5 ketones, 3 alcohols, and 9 other compounds. This comprehensive and systematic qualitative analysis of the chemical constituents of Anisi Stellati Fructus provides a solid foundation for further research on its pharmacodynamic material basis, quality control, and pharmacological mechanisms.