Along with the discoveries of carbon nanotube, fullerenes, and graphene, 1,2 the insight on the properties of carbon nanomaterials has been greatly promoted, and carbon nanomaterials have been applied to various fields such as energy, environment, and materials based on their unique nanostructure and properties. 3‐7 As the results, the applications of these known materials not only enrich the knowledge of carbon nanomaterials but also encourage the expectation of other novel carbon nanomaterials. Graphite, a basic carbon material and the raw material of carbon nanomaterials, has been largely used as the active material in the anodes of lithium ion batteries (LIBs) recently. Although the annual output of LIBs has increased quickly and their cathode materials are generally recycled, 8,9 the waste graphite anode materials are usually abandoned because of the knowledge lack on their recovery value. In practice, the status quo on the incessant accumulation of spent anode active materials can’t be neglected from the environmental viewpoint, and the remnant lithium in the active materials must also be considered, showing the essentiality to reclaim the graphite in spent LIBs. Because the perfect layered structure of spent graphite has been changed and an uncertain amount of lithium ions remain in the graphite lattice voids, the reusing of spent graphite, even after a regeneration, as the anode active material of LIBs is impossible. In addition, the uncertainty for the lifetime and states of the spent LIBs collected from different resources has to be faced, which also puzzles the reclaiming of the graphite anodes in spent LIBs. Recently, we prepared a novel carbon nanomaterial that is denoted as carbon nano-fragments (CNFs) by using the graphite in spent LIBs as raw material. And this CNFs material exhibits some similar properties to carbon nanotube and graphene 10,11 and excellent electrocatalytic oxidation activity to organic molecules such as dopamine, β-cyclodextrin, and phenol, showing potential application in the electrochemical fields. In this paper, the preparation and the characterization on the morphology, structure, functional groups, and electrocatalytic activity of the as-prepared CNFs are presented.