Electrochemically exfoliated graphene (EEG) is a new generation of high-quality graphene that holds, great promise for the construction of hyhrid materials. However, the assembly of EEG hybrids with well-defined nanostructures has remained a major challenge. In this study, we demonstrate a bottom-up approach toward the assembly of EEG sheets with a series of functional nanoparticles (Si, Fe3O4, and Pt NPs) into two-dimensional Sandwich-like hybrid nanostructures. Polyaniline in the emeraldine base form functions as a: versatile dopant to Couple NPs :onto EEG through,either electrostatic interactions or hydrogen, bonding. This protocol enables processing and assembly of BE using an economical pathway, for which we further demonstrate the potential application of EEG-Si hybrids as high-performance anode material for lithium storage.