Abstract: ²⁷Al is the only stable isotope of aluminum, is an odd-proton nucleus. The energy level information of its ground and excited states helps test the predictive power of nuclear models, such as the shell model and collective models (e.g., rotational and vibrational models). Its level transition properties also provide insights into the collective and single-particle behavior of nucleons, aiding in the understanding of nuclear deformation. On the other hand, Al plays a significant role in other fields, such as nuclear astrophysics and gamma-ray astronomy. Studying nuclear reactions involving ²⁷Al requires a thorough understanding of its excited-state level structure, particularly near the reaction threshold, it is now crucial to determine the spectroscopic information of ²⁷Al, such as spin-parity assignments. In this work, the angular distributions of the proton transfer reaction ²⁶Mg(⁷Li, ⁶He)²⁷Al were measured using the HI-13 Tandem Accelerator and a high-precision Q3D magnetic spectrograph. Previous international studies have rarely investigated the (⁷Li, ⁶He) transfer reaction system. This reaction provides unique capabilities for populating excited states that are difficult to measure via other transfer reactions or direct reactions. Furthermore, our research group’s accumulated experimental results using this reaction system have consistently demonstrated both its reliability and unique scientific merit. In the same time, this also marks the first measurement of this reaction using the indirect proton-transfer method with ⁷Li, providing complementary data to previous results obtained via ³He proton transfer and direct measurements. Importantly, this approach may populate excited states in ²⁷Al that are inaccessible through conventional ³He-induced reactions, representing a significant exploratory study of ²⁷Al excited states. Additionally, elastic scattering measurements were conducted for the entrance channel to extract the optical potential in the Woods-Saxon form. To eliminate other potential influences, single-folded potentials were also employed to fit the angular distributions of the entrance channel as a cross-check. For the exit channel, since no elastic scattering data were measured in this experiment, two sets of elastic scattering angular distributions from neighboring nuclei in the literature were used for extraction. Through the aforementioned approach, potential influences of optical potential selection on the final results have been minimized. The final uncertainty in the optical potential was determined by averaging the results from multiple sets of optical potentials. By analyzing the angular distributions with the distorted wave Born approximation (DWBA) method and FRESCO code, the proton spectroscopic factors for three states were extracted and their transferred angular momenta and parities were determined. For the excited state at 9080 keV, the analysis of the angular distributions suggests a spin-parity assignment that differs from the one listed in the National Nuclear Data Center. Compared to conventional direct measurements and indirect approaches using (³He, d) or (d, n) transfer reactions, the (⁷Li, ⁶He) reaction system offers unique advantages. It provides complementary constraints to other experimental studies and can help resolve discrepancies, particularly for uncertain level information. Future work will employ this reaction to investigate energy levels of additional key nuclides.