Hydrogen is regarded as an attractive substitute for fossil fuel, but stable and safe storage of hydrogen remains a formidable challenge. In this work, a nanometer-thickness Mg nanosheet is synthesized in a one-pot system for the first time and it enables expedited hydrogen sorption through its large surface area and shortened transport paths. The Mg nanosheets absorb about 6 wt % hydrogen within 1 h without any catalyst. Also, it is demonstrated that upon adding one-dimensional carbon materials, Mg nanosheet exhibits enhanced performance with temperature-dependent characteristics due to the interaction between edge site carbon of graphite nanofiber and Mg.