According to the fact that gecko-inspired vertically aligned carbon nanotubes (VA-CNTs) exhibit ultrastrong adhesion, dopamine is utilized to make a modification to this traditional biomimetic material. The composite material is tested for adhesion performance under different environmental conditions by an atomic force microscope. The adhesion force of the modified VA-CNTs does not show obvious fluctuation during the gradual heating process; however, the material gains improved adhesion when increasing the ambient humidity. In addition, the modified CNTs show a stronger adhesion force than the original CNTs in their performance tests. The dopamine polymer has a good combination with CNTs, which is responsible for the aforementioned excellent performance. Overall, this modification method is simple, convenient, efficient, and environmentally friendly, which all indicates a promising future in its application. The modified CNTs are expected to be used for super-adhesion in harsh environments, as well as in the field of microelectronics.