In the present work, we have synthesized and studied the catalytic effect of different carbon nanostructures (CNSs) on the absorption kinetics, decomposition temperature of MgH2. Ball-milling was used to reduce the particle size of MgH2 and CNS catalysts were used to enhance the hydrogen storage properties at lower temperatures. In particular, 2wt% twisted carbon nanofibres (TCNF) admixed ball-milled MgH2 (MgH2-2TCNF) corresponds to better hydrogenation/ dehydrogenation behaviour. The commencement of H-desorption temperature is ∼420 ?C for pure MgH2, ∼ 330 °C for TCNF admixed MgH2, which is further lowered to 297 °C for TCNF admixed ball-milled MgH2. Thus, desorption temperature gets more than 125 °C lower compared to commercial MgH2. After the desorption, Mg- 2TCNF (ballmilled) shows 5.03 wt% absorption as compared to 3.05 wt% for the ball milled MgH2 in the first 10 minutes even at 180 °C and an applied pressure of 2MPa. Whereas in the case of 2TCNF admixed MgH2 it shows absorption of 4.28 wt% at a higher temperature 300 °C and an applied pressure of 2 MPa. The improved properties originate due to the CNSs catalyst and nanostructure of MgH2 introduced during ball milling in hydrogen pressure.