MgH2 has been attracted extensive attention because of its superior hydrogen storage performance and good reversibility. Further improvement of its kinetics and thermodynamic performances is needed to achieve widespread application. This article investigated the hydrogen storage properties of the thermodynamic optimized Mg-TiCrV hydrogen storage composite modified by layered Ti3C2 materials containing different 3d transition metal particles (Fe, Co, Ni). Mg-TiCrV/Ti3C2-X (X = Fe, Co, Ni) composites can absorb more than 5.30 wt% hydrogen within 1 min at 453 K under 3 MPa hydrogen pressure, and desorb more than 5.25 wt% hydrogen within 60 min at 543 K to 0.1 MPa. In particular, Mg-TiCrV/Ti3C2-Ni composite exhibited the best hydrogen storage properties, which can desorb 4.98 wt% hydrogen within 60 min at 523 K to 0.1 MPa hydrogen pressure and absorb 5.80 wt% hydrogen within 1 min at 453 K under 3 MPa hydrogen pressure. Structural analysis shows that the synergistic effect of layered material Ti3C2 and Ni particles promote the hydrogen release and uptake process.