Exfoliated graphite oxide (GO) sheets with hydroxyl groups and amine groups on the surface were prepared by modification of graphite. Atom transfer radical polymerization (ATRP) initiator molecules were grafted onto the GO sheets by reactions of 2-bromo-2-methylpropionyl bromide with hydroxyl groups and amine groups. Poly(2-(dimethylamino)ethyl methacrylate) (PDMAEMA) chains oil the surface of GO sheets were synthesized by in-situ ATRP. X-ray photoelectron spectroscopy, thermogravimetric analysis, and transmission electron microscopy (TEM) results all demonstrated that polymer chains were successfully produced. After grafting of PDMAEMA, the dispersity of GO sheets in solvents was improved significantly. Poly(ethylene glycol dimethacrylate-co-methacrylic acid) particles were deposited on GO sheets via hydrogen bonding between MAA units on polymer particles and airline groups of PDMAEMA. TEM and scanning electron microscopy were used to characterize the structure of the nanocomposites.