Graphene-coated polymer particles have attracted research interests due to their emerging applications derived from their controlled structure and morphology. To control the properties of graphene oxide (GO)-polystyrene (PS) composite particles, the adsorption time and instantaneous adsorption conditions were investigated by varying their mixing method. Polystyrene particles prepared by emulsion polymerization were modified to have positive surface charge by adsorption of polyethylene imine (PEI) on the surface of PS particles. GO prepared by the chemical exfoliation method had negative surface charge from the oxygenated groups. The adsorption of the negatively charged GOs onto the positively charged PS particles was successfully completed, and it was found that a longer adsorption time and a greater difference in the instantaneous relative concentration led PS-GO particles to have more homogeneously coated surfaces without aggregation.