Nano-compounds of ZrO2/CNTs were prepared by hydrothermal method. The ZrO2/CNTs nano-compounds were characterizated by XRD, TEM, BET and Zeta potentials. The results showed that perfect hydrothermal temperature was 180°C, hydrothermal time was 11h, pH was 9.5. It is showed by the analysis of TEM and Zeta potential, adding surfacant CTBA, the surface of nano-tube and Zr(OH)4 colloids take different charge, and they adsorpt each other. And ZrO2 particles were successfully coated on the CNTs in surface-active agent of CTBA.