For decades, the nanostructure of carbon nanotubes (CNTs) have attracted ample attention in the application of gas sensors. However, those CNT-based gas sensors are mostly manufactured in the single or film structures. Until now, the CNT bundle structure in gas sensors has not yet been investigated by researchers. In this study, the effects of the film and the bundle structure in CNTs are explored. The abundant interstitial and groove sites, beneficial for N_2 gas absorption and charge transfer, were provided through the CNT bundle with particular geometric structures. In terms of detecting nitrogen gas, the CNT bundle is found to have significantly superior sensitivity, faster response and recover time, comparing to the CNT film. Therefore, the geometric structure of CNTs is approved to be one of the features the designers of the gas sensor should take into consideration in the future.