Carbon nanotube (CNT) sensors provide a versatile chemical platform for ambient monitoring of ozone (O3) and nitrogen dioxide (NO2), two important airborne pollutants known to cause acute respiratory and cardiovascular health problems. CNTs have shown great potential for use as sensing layers due to their unique properties, including high surface to volume ratio, numerous active sites and crystal facets with high surface reactivity, and high thermal and electrical conductivity. With operational advantages such as compactness, low-power operation, and easy integration with electronics devices, nanotechnology is expected to have a significant impact on portable low-cost environmental sensors. Enhanced sensitivity is feasible by functionalizing the CNTs with polymers, metals, and metal oxides. This paper focuses on the design and performance of a two-element array of O3 and NO2 sensors comprising single-walled CNTs functionalized by covalent modification with organic functional groups. Unlike the conventional chemiresistor in which the change in DC resistance across the sensor terminals is measured, we characterize the sensor array response by measuring both the magnitude and phase of the AC impedance. Multivariate response provides higher degrees of freedom in sensor array data processing. The complex impedance of each sensor is measured at 5 kHz in a controlled gas-flow chamber using gas mixtures with O3 in the 60–120 ppb range and NO2 between 20 and 80 ppb. The measured data reveal response change in the 26–36% range for the O3 sensor and 5–31% for the NO2 sensor. Multivariate optimization is used to fit the laboratory measurements to a response surface mathematical model, from which sensitivity and selectivity are calculated. The ozone sensor exhibits high sensitivity (e.g., 5 to 6 MΩ/ppb for the impedance magnitude) and high selectivity (0.8 to 0.9) for interferent (NO2) levels below 30 ppb. However, the NO2 sensor is not selective.