The cryogenic ball milling was performed on carbon nanotubes (CNTs) at an extremely low temperature to increase the dispersion of CNTs. The effects of milling speed and time on the deagglomeration and structural changes of CNTs were studied. FESEM was used to analyze the dispersion and the change of particle size before and after milling process. Transmission electron microscopic (TEM) analysis was also investigated the effect of cryogenic ball milling on the morphological characteristics of CNTs. The structural changes by the cryogenic ball milling process were further confirmed by x-ray diffraction (XRD) and Raman spectroscopic analysis. The results showed that the agglomeration of CNTs was significantly reduced and amorphous structure was observed at high milling speed. However, the milling time has no great effect on the dispersion property and structural change of CNTs compared with milling speed.