Countless organisms in nature have adapted high-aspect-ratio micro-/nano-fibrillar arrays on their functional surfaces for achieving special and often optimized functionalities using earthly abundant materials. At the core of nanoscience and nanotechnology, rationally mimicking nature offers a promising route to create multifunctional superstructures that capture organisms and biological materials’ intriguing responsive and self-adjusting properties. Prior work has demonstrated that hierarchical vertically aligned multi-walled carbon nanotube (VA-MCNT) arrays can achieve ten folds of adhesive force comparing to the fibrillar structures of the gecko toe pads. However, little is known with regard to their wettability at the ultimate atomistic level, and how this may influence the adhesive performance and/or self-cleaning capabilities, despite water condensation and bridging are common phenomena at this length scale. In present study, molecular dynamics (MD) simulations were performed using Large-Scale Atomic / Molecular Massively Parallel Simulator (LAMMPS). Results indicate that commonly believed hydrophobic defect free CNTs (i.e., carbon sp2 hybridization without any dangling bonds) become super-hydrophilic at this length/temporal scale. The critical factors that influence the number of H-Bonds in water are: i) tube-tube spacing; and ii) shape/size and position of the water nanodroplet; and iii) how many droplets exists and how many nanotubes are bridged by the droplets. Chirality has little effect on the water interfacial behaviors. Future work will focus on the effect of water condensation and bridging on the adhesive and self-cleaning properties of carbon-based bio-inspired fibrillar dry adhesives considering defects and saline water.