Different ionic liquid modified graphene nanosheets (IG) were induced into polyimide (PI) to improve the tribological, thermal, and mechanical properties of shape memory IG/PI composites. The results demonstrated that when using 1-aminoethyl-3-methylimidazole bromide to modify graphene nanosheets (IG-1), the laser-driven shape recovery rate of IG-1/PI composites (IGPI-1) reached 73.02%, which was 49.36% higher than that of pure PI. In addition, the IGPI-1 composite materials reached the maximum shape recovery rate within 15 s. Additionally, under dry sliding, the addition of IG can significantly improve the tribological properties of composite materials. IGPI-1 exhibited the best self-lubricating properties. Compared with pure PI, the friction coefficient (0.19) and wear rate (2.62 × 10–5) mm3/Nm) were reduced by 44.1% and 24.2%, respectively, and the T10% of IGPI-1 increased by 32.2°C. The Tg of IGPI-1 reached 256.5°C, which was 8.4°C higher than that of pure PI. In addition, the tensile strength and modulus of IGPI-1 reached 82.3 MPa and 1.18 GPa, which were significantly increased by 33.6% and 29.8%, respectively, compared with pure PI. We hope that this work will be helpful for the preparation of shape memory materials with excellent tribological, thermal, and mechanical properties.