Graphene nano-sheets (GNs) with high quality were successfully synthesized in a Teflon-lined container through a low temperature expansion process. The influence factors of expansion temperature, expansion mode and reduction time on the morphology and structure of products have been systematically investigated, and an optimum experimental condition for the synthesis of GNs has been obtained. The results showed that the Teflon-lined container is an effective apparatus for preparing GNs at relative low temperature (<300 °C). The low temperature synthetic process is simple, inexpensive and easy to scale up in comparison with the traditional method which often consume more energy, use more complicated instruments, or more costly. The electrochemical properties of the as-synthesized products were investigated as anode materials for lithium ion batteries.