Poor air quality (PAQ) is a global concern, especially in urban areas, and is often seen as an important element of social sustainability given its negative impact on health and quality of life. However, little research has been undertaken in cities of the developing world to explore how residents perceive poor air quality, its main causes, what control measures should be used to address PAQ and where the main responsibility rests for implementing control measures. The research described in this paper sought to address these points, using a questionnaire-based survey (n = 262) in Nigeria’s federal capital city of Abuja (n = 137) and the state-capital city of Enugu (n = 125). The survey took place during the COVID-19 pandemic (October 2020 to March 2021), and was stratified to ensure representation across a number of demographic groups such as gender, age, education and income. The results were analysed using the Kruskal–Wallis non-parametric test and Hochberg’s post hoc test available in SPSS version 28. The study found that the ranking of perceptual indicators and the main causes of PAQ had much agreement between respondents from both cities and between demographic groups. Smoke, odour and dust particles were perceived to be the most important indicators of PAQ, while the main sources of PAQ were waste and bush burning, vehicle use and power generators. The two most preferred control measures were proper waste management and the avoidance of bush burning. However, there was a significant difference between the two cities in terms of the main organisations responsible for addressing PAQ, with respondents from Abuja citing the federal government, while those from Enugu cited the state government. Interestingly, younger people in Enugu noted that the government should take more responsibility in controlling PAQ than did the older demographic in that city, but this difference was not seen in Abuja. Overall, this study reveals that residents in these two Nigerian cities clearly recognise their exposure to PAQ and it suggests that these perceptual indicators, and views on sources and interventions should be central to designing policies to control this important issue.