Abstract: LiAlH4 is hindered for practical hydrogen storage by its high decomposition temperatures, slow kinetics, and poor reversibility. To address the kinetic issues, this study introduces a tubular g-C3N4-supported NiFe-layered double hydroxide (g-C3N4@NiFe-LDH) nanocomposite as a catalytic dopant for LiAlH4. The composite, synthesized via solvothermal and pyrolysis methods, features a well-defined tubular morphology (∼3 μm in length, ∼200 nm in diameter), which facilitates its homogeneous dispersion and intimate interfacial contact with LiAlH4 during ball milling. Doping with 7 wt% of this catalyst dramatically enhances the dehydrogenation kinetics of LiAlH4. The onset dehydrogenation temperature is lowered to 79.2°C, and 6.76wt% of hydrogen is released in two steps. Kissinger analysis reveals that the apparent activation energies for these steps are reduced by 43.0% and 54.8%, respectively, demonstrating significantly improved dehydrogenation kinetics. Mechanistic studies suggest that the synergistic effect between the g-C3N4 support and NiFe-LDH, along with the potential in-situ formation of active interfacial species during dehydrogenation, contributes to this improvement.