The air quality (AQ) in urban contexts is a major concern, especially in the developing world. The environmental and social challenges created by poor AQ have continued to increase despite improvements in monitoring AQ using earth observation (EO) satellites, static and mobile ground-based sensors and models. However, these types of equipment can be expensive to purchase, operate, and maintain, especially for cities of the developing world, and, as a result, there is growing interest in the elicitation of residents’ perceptions of AQ. However, there is a need to analyse how the results obtained from sensor measurements and models match the AQ as perceived by residents. This study explored AQ in multiple locations in two developing world cities (Abuja and Enugu) in Nigeria by analysing the perceptions of 262 residents and how these compared with findings obtained from ground-based instruments. The results suggest that the perceived AQ of the locations broadly matches those obtained using instruments, although there were statistically significant differences between respondent groups based on the demographic factors of income-education (Abuja) and age (Enugu). This research supports the contention that perceptual AQ assessment provides a valuable source of data for policy and decision-makers when addressing poor AQ and can support action in the absence of instrument-based measurements.