In this work, the evolution of mechanical properties of binary Al–Li alloys with four approximately equal gradient Li contents (0.91–3.98 wt.%) under aging conditions is thoroughly investigated. The alloys undergo aging treatments at 175 °C for x hours (x = 0–120 h), and the peak-aged times of the four alloys are 6 h, 12 h, 48 h and 48 h, respectively, as the Li concentration increases. Both in the solution-treated and peak-aged states, the elastic modulus of binary Al–Li alloys exhibits an approximately linear increase with increasing Li content, consistent with trends predicted by density functional theory (DFT) calculations. Due to the presence of Al3Li precipitates, the modulus of higher-Li-concentration alloys in the peak-aged state increases by approximately 1.4–2.5% compared with that of alloys in the solution-treated state. Additionally, the study finds that increasing Li content significantly enhances the tensile strength and yield strength of the alloy but decreases its ductility, leading to a transition in fracture mode from ductile to brittle, as evidenced by a microscopic analysis of fracture surfaces. Under peak-aged (175 °C/48 h), the alloy with the highest Li content exhibits the maximum tensile strength of 341 MPa and a yield strength of 296 MPa, while its elongation is the lowest at 2.1%. These findings contribute to a deeper understanding of the effects of aging precipitates on the mechanical properties of Al–Li alloys, providing fundamental guidance for the design of future generations of Al–Li alloys.