This paper clarifies the contribution of lactones and volatile phenols to the aroma of nongrape wine. A target method for the simultaneous determination of these two kinds of volatiles in nongrape wines was developed using headspace-solid-phase microextraction (HS-SPME) combined with high-resolution gas chromatography-Orbitrap mass spectrometry (GC-Orbitrap-MS). A high-resolution mass spectrometry database including 12 lactones and 11 volatile phenols was established for qualitative accuracy. Different matrix-matched calibration standards should be prepared for specific samples due to the matrix effects. The method was successfully validated and applied in three nongrape wines. Hawthorn wine contained more lactones (δ/γ-hexalactone, δ/γ-nonalactone, δ/γ-decalactone, γ-undecalactone, δ/γ-dodecalactone, C10 massoia lactone, and whiskey lactone), while blueberry wine contained more volatile phenols (especially 4-vinylguaiacol and 4-ethylguiaiacol). Goji berry wines contained certain concentrations of δ-nonalactone, γ-nonalactone, δ-hexalactone, and 3-ethyl phenol. This study demonstrated that HS-SPME-GC-Orbitrap-MS can be applied for the accurate quantification of trace aroma compounds such as lactones and volatile phenols in fruit wines.