Carbon spheres were rapidly synthesized at low temperature (300 °C) via the chemical metathesis reaction between CaC2, C2Cl4, and CCl4. X-ray diffraction and Raman results confirm the formation of hexagonal graphite with relatively low graphitization. Large quantities of carbon spheres can be observed by transmission electron microscopy in the products obtained within the reaction temperature range of 300−480 °C. The spheres with a surface area of 195.28 m2/g have a hydrogen storage capacity of 3.8 wt % at room temperature under a pressure about 10 MPa. The synergic carbon sources are likely responsible for the formation of the carbon spheres.