In this study, the rolling process of the warm-rolled duplex-phase Mg–8.3Li–3.1Al–1.09Si alloy and the strengthening mechanism of as-rolled Mg–Li alloy were investigated. The highest ultimate tensile strength (UTS, 323.66 ± 19.89 MPa) could be obtained using a three-pass rolling process with a 30% thickness reduction for each pass at 553 K. The strength of the as-rolled LAS831 alloy is determined by a combination of second-phase strengthening, grain refinement strengthening, dislocation strengthening, and load-transfer reinforcement. Of these factors, dislocation strengthening, which is caused by strain hardening of the α-Mg phase, can produce a good strengthening effect but also cause a decrease in plasticity. The Mg2Si phase is broken up into particles or strips during the rolling process. After three passes, the AlLi particles were transformed into an AlLi phase, and the Mg2Si particles and nanosized AlLi particles strengthened the second phase to form a hard phase. The average size of the DRXed β-Li grains decreased with each successive rolling pass, and the average size of recrystallized grains in the three-pass-rolled LAS831 alloy became as low as 0.27 μm. The interface between the strip-like Mg2Si phase and the α-Mg phase is characterized by semicoherent bonding, which can promote the transfer of tensile and shear forces from the matrix to the strip-like Mg2Si phase, thereby improving the strength of the matrix and thus strengthening the LAS831 alloy.