Aggregation and weak interfacial bonding limit the superior strengthening potential of the carbon nanotubes (CNTs) in the metal matrix composites. To overcome these challenges, in situ Mg2Si nanoparticles (Mg2Sip) have been hybridized with surface modified CNTs through chemical oxidization. The synergistic strengthening was enhanced by tailoring the volume ratios of CNTs to Mg2Sip in the Mg matrix through powder thixoforming technology. Herein, when 0.3CNTs-1.2Mg2Sip was added, a yield strength, ultimate tensile strength, and elongation of 213 MPa, 271 MPa, and 6.3%, respectively, were obtained, which were 18.3%, 16.8%, and 3.3% higher than those of the 0.75CNTs-0.75Mg2Sip/Mg composites, respectively. The strengthening effects of the CNTs-Mg2Sip reinforcements were more effective than those of the individual 1.5CNTs and 1.5Mg2Sip owing to the effective thermal mismatch and load transfer strengthening mechanisms. In this study, we propose an effective approach to harness the superior performances of the hybrid reinforcements for enhancing the composites.