Flexible, water-resistant, and air-stable hydrogen storage material (named PMMA-LiBH 4 /GMF), consisting of LiBH 4 nanoparticles confined by poly (methylmethacrylate) (PMMA) and reduced graphene oxide (rGO) modified melamine foam (GMF), were prepared by a facile method. PMMA-LiBH 4 /GMF can recover original shape after compression at the strain of 50% and exhibits highly hydrophobic property (water contact angle of 123 •). Owing to the highly hydrophobic property and protection of PMMA, PMMA-LiBH 4 /GMF demonstrates outstanding water-resistance and air-stability. Significantly, the onset dehydrogenation temperature of PMMA-LiBH 4 /GMF at first step is reduced to 94 • C, which is 149 • C less than that of LiBH 4 /GMF, and the PMMA-LiBH 4 /GMF desorbs 2.9 wt% hydrogen within 25 min at 250 • C, which is obviously more than the dehydrogenation amount of LiBH 4 /GMF under the same conditions. It's our belief that the flexible, water-resistant and air-stable PMMA-LiBH 4 /GMF with a simple preparation route will provide a new avenue to the research of hydrogen storage materials.