Graphene quantum dots modified nanoporous SiAl (NP-SiAl/GQDs) composite was easily prepared by a facile dealloying followed by the encapsulation of graphene quantum dots. Nanoporous Si with part of Al residues was first fabricated through incomplete corrosion of binary Si5Al95 precursor alloy. GQDs were then used as the building units to enwrap the positively charged NP-SiAl on the basis of the electrostatic assembly. Owing to the combination of graphene quantum dots and embedded Al, NP-SiAl/GQDs displays dramatically boosted lithium storage performances with excellent reversible capacity, outstanding cyclability, as well as high rate capability. Especially, NP-SiAl/GQDs composite exhibits superior cycling stability with large reversible capacity of 1318.7 and 1005.5 mAh g−1 retained after 120 and 150 cycles under the rate of 200 and 1000 mA g−1, respectively. Moreover, it exhibits high reversible capacity even cycled at 3000 mA g−1. With the merits of facile preparation and exceptional performances, the as-prepared NP-SiAl/GQDs composite presents great application potential as next-generation anode material in lithium ion batteries.