Carbon nanotubes (CNTs) were synthesized by thermal chemical vapor deposition (thermal CVD) on n-type Si (100) at 700 ° under C2H2 gas flow ratio of 30 sccm. Fe catalysts were pre-deposited by RF sputtering system with RF power 150 W. Two kinds of as-grown CNTs were used to detect N2: the vertically oriented carbon nanotubes (CNTs) mat and horizontally oriented CNTs bundle. Two-terminal electrical measurements were performed at room temperature of 25 °. The electrical resistance of CNTs mat or bundle was found to increase when exposed to N2 environment, and to return back after the N2 pumping, respectively. However, the CNTs bundle had better sensitivity and possessed faster response and recovery time. This could be ascribed to that the CNTs bundle, with more effective grooves on the surface, provided more lower binding-force sites to absorb N2 molecules than the CNTs mat dose, which prominently had interstitial sites.