We demonstrate highly sensitive and selective chemiresistive-type NO gas detection using defected single-walled carbon nanotubes (SWCNTs) decorated with N-[3-(trimethoxysilyl)propyl]ethylene diamine (en-APTAS) molecules. The defected SWCNTs were prepared via furnace annealing at 700 °C and confirmed by transmission electron microscopy. A single en-APTAS molecule has two amine groups acting as adsorption sites for NO gas, which can improve the NO response. The NO response was further enhanced when the defected SWCNTs were utilized because NO sensing reactions could occur on both the inner and outer walls of the defected SWCNTs. The en-APTAS decoration improved the NO response of the SWCNT-based gas sensing devices by 2.5 times; when the defected SWCNTs were used, the NO response was further improved by 3 times. Meanwhile, the recovery performance in a time-resolved response curve was significantly improved (45 times) via a simple rinsing process with ethanol. Specifically, the fabricated device did not respond to carbon monoxide (CO) or BTEX gas (i.e., a mixture of benzene, toluene, ethyl benzene, and xylene), indicating its high selectivity to NO gas. The results show the possibility of a high-performance SWCNT-based NO gas sensor applicable to healthcare fields requiring ppb-level detection, such as in vitro diagnostics (IVDs) of respiratory diseases.