This study provides valuable insights into two key areas. First, we conduct a detailed examination of aluminum nitride nanotubes (AlNNT (m,n)_k), where m = 5,7; n = 0,5,7; and k = 3−9, focusing on their electronic properties across different lengths and diameters. We then investigate how these nanotubes interact with various gases, including CO, CO2, NO, NO2, and SO2. To determine the most energetically favorable configurations, we use the bee colony algorithm for global optimization. Our computational approach employs several Density Functional Theory (DFT) methods, such as PBE0, B3LYP(GD3BJ), CAM-B3LYP, HSE06, M06–2X, TPSSh, and ωB97XD functionals, in combination with the Def2svpp basis set. We prioritize the optimization of structural configurations and analyze the changes in energy band gaps within the nanotubes using conceptual DFT analysis. Additionally, we examine charge transfer mechanisms during gas/nanotube interactions through Natural Bond Orbital (NBO) analysis and assess the nature of these interactions with the Quantum Theory of Atoms in Molecules (QTAIM) framework. Our findings reveal that the interaction with SO2 tends to be slightly stronger compared to the other gases, as evidenced by various analytical techniques. This comprehensive analysis enhances our understanding of gas interactions with aluminum nitride nanotubes and provides insights into their practical applications.