Professor Zaifa Shi's team at Xiamen University developed an ultra-high temperature flash vacuum pyrolysis (UT-FVP) device to form giant fullerenes from single-carbon molecules within a short time (15 s) at extremely high temperatures (∽3000 ℃). Due to the strong intermolecular forces between giant fullerene molecules and soot, traditional ultrasonic or Soxhlet extraction methods cannot separate most giant fullerenes from soot in toluene. To overcome these strong intermolecular forces, two separation techniques—mechanical grinding and sublimation—were optimized to separate the giant fullerenes from the pyrolysis products, and laser desorption/ionization time-of-flight mass spectrometry (LDI-TOFMS) was used for comprehensive and thorough detection. These methods extended the mass distribution of synthesized giant fullerenes to 2760 Da (greater than C₂₃₀). Notably, the separation technology can also recover giant fullerenes that have long been neglected due to incomplete separation in flame and arc discharge methods. This separation strategy has broad applicability in the synthesis of giant fullerenes, providing a new perspective for the synthesis and utilization of these carbon materials. The article was published as an open access research article in CCS Chemistry, the flagship journal of the Chinese Chemical Society.