The effects of mold temperatures on the microstructures and mechanical properties of thixoforged Grp (graphite particles)/AZ91D composites have been investigated, followed by partial remelting and thixoforging technology. The results indicate that the best semi-solid microstructure could be obtained after being partially remelted at 600 °C and held for 60 min. Correspondingly, under a mold temperature of 300 °C, the best tensile properties were obtained by thixoforging. The UTS (ultimate tensile strength) and elongation of the thixoforged Grp/AZ91D were up to 304.1 MPa and 13.9%, respectively, which increased 11.3% and 43.1% in comparison with the thixoforged AZ91D, respectively. The variation of the tensile properties responded to the influences of mold temperatures on the amount of eutectic phase, the distribution of Grp, and the grain size of α-Mg. Meanwhile, HRTEM (High Resolution Transmission Electron Microscope) showed good bonding between Grp and AZ91D, and many edge dislocations were found in the inverse FFT (Fast Fourier Transform) image. And the result showed that the increase in tensile properties is attributed to the synergistic effect of load transfer, dislocation strengthening, and Orowan looping mechanisms from the Grp strengthening the matrix.