Vertically-aligned carbon nanotubes (VACNTs) have extraordinary structural and mechanical properties, and have been considered as potential candidates for creating dry adhesives inspired by adhesive structures in nature. Catalytic chemical vapor deposition is widely used to grow VACNTs; however, the influential mechanism of VACNT preparation parameters (such as H 2 concentration) on its adhesion property is not clear, making accurate control over the structure of VACNTs adhesive an ongoing challenge. In this article, we use electron beam-deposited SiO 2 /Al 2 O 3 as a support layer, Fe as catalyst, and C 2 H 4 /H 2 gas mixtures as a feed gas to prepare VACNTs, while varying the ratio of the reducing atmosphere (H 2 ) from 0% to 35%. VACNTs synthesized at a 15% H 2 concentration (5 mm × 5 mm in size) can support a maximal weight of 856 g, which indicates a macroscopic shear adhesive strength of 34 N/cm 2 . We propose a hydrogen-concentration-dependent model for the shear adhesive performance of VACNTs. By adjusting the amount of hydrogen present during the reaction, the morphology and quality of the prepared VACNTs can be precisely controlled, which significantly influences its shear adhesive performance. These results are advantageous for the application of carbon nanotubes as dry adhesives.