Based on the re-construction idea of carbon nanomaterials, novel folding re-constructed carbon nanosheets (re-CNSs) with unique microstructure and higher lithium-ion storage capacity than prototype graphite powders are prepared. The nanoscale carbon-fragment suspension is firstly prepared through a successive chemical oxidation of graphite and ultrasonic crushing operation, and the re-CNS powders are then obtained by spray drying the suspension and a subsequent high-temperature reducing process. The as-prepared re-CNSs exhibit a folding appearance with a width of several micrometers, with a maximum initial specific capacity of 903mAhg−1 for the re-CNSs sample thermally reduced at 500°C (re-CNSs500). After 100 cycles, the reversible capacity is maintained at about 400mAhg−1 for the re-CNSs500. The abundant carboxylic and hydroxide groups, edges, and defective sites of individual graphite oxide fragments facilitate the dislocation formation in the re-CNSs. In addition, a dislocation mechanism is thus used to describe the enhanced lithium-ion storage.