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Multi-walled carbon nanotubes (MWCNTs) with large inner diameter were synthesized by the catalytic chemical vapor deposition method using HBO₃ as the accessorial catalyst in reaction precursors. A ratio Dᵢₙ/Dₒᵤₜ is defined as an index to evaluate the hollow degree of MWCNTs, where Dᵢₙ and Dₒᵤₜ are the inner and outer diameter of one CNT, respectively. When no HBO₃ was added in the reaction mixtures, the MWCNTs are straight with thick wall. The average Dᵢₙ/Dₒᵤₜ value is only 0.08±0.02. The X-ray diffraction (XRD) result shows the relatively low crystallinity. When HBO₃ was added in the reaction precursors, the MWCNTs have large inner cavity and the average Dᵢₙ/Dₒᵤₜ value reaches 0.57±0.10. The crystallinity was also improved remarkably. These results indicate that HBO₃ in the catalyst system has great influence on the growth of MWCNTs.