Low defect concentration few-layer graphene (FLG) sheets were fabricated by a two-step electrochemical intercalation exfoliation, including a graphite foil pretreatment in sodium hydroxide solution and a subsequent further exfoliation in sulfuric acid solution. During the process, the pretreatment results in the expansion of the graphite foil and in turn facilitates the final exfoliation in sulfuric acid solution. The results show that the I(D)/I(G) of the obtained FLG sheets is as low as 0.29 while maintaining relatively high yield, more than 56%. In addition, the oxygen content in the FLG sheets is 8.32% with the C/O ratio of 11.02.