The megacities experience poor air quality frequently due to stronger anthropogenic emissions. India had one of the longest lockdowns in 2020 to curb the spread of COVID-19, leading to reductions in the emissions from anthropogenic activities. In this article, the frequency distributions of different pollutants have been analysed over two densely populated megacities: Delhi (28.70° N; 77.10° E) and Kolkata (22.57° N; 88.36° E). In Delhi, the percentage of days with PM
2.5
levels exceeding the National Ambient Air Quality Standards (NAAQS) between 25 March and 17 June dropped from 98% in 2019 to 61% in 2020. The lockdown phase 1 brought down the PM
10
(particulate matter having an aerodynamic diameter ≤ 10 μm) levels below the daily NAAQS limit over Delhi and Kolkata. However, PM
10
exceeded the limit of 100 μgm
−3
during phases 2–5 of lockdown over Delhi due to lower temperature, weaker winds, increased relative humidity and commencement of limited traffic movement. The PM
2.5
levels exhibit a regressive trend in the highest range from the year 2019 to 2020 in Delhi. The daily mean value for PM
2.5
concentrations dropped from 85–90 μgm
−3
to 40–45 μgm
−3
bin, whereas the PM
10
levels witnessed a reduction from 160–180 μgm
−3
to 100–120 μgm
−3
bin due to the lockdown. Kolkata also experienced a shift in the peak of PM
10
distribution from 80–100 μgm
−3
in 2019 to 20–40 μgm
−3
during the lockdown. The PM
2.5
levels in peak frequency distribution were recorded in the 35–40 μgm
−3
bin in 2019 which dropped to 15–20 μgm
−3
in 2020. In line with particulate matter, other primary gaseous pollutants (NO
x
, CO, SO
2
, NH
3
) also showed decline. However, changes in O
3
showed mixed trends with enhancements in some of the phases and reductions in other phases. In contrast to daily mean O
3
, 8-h maximum O
3
showed a reduction over Delhi during lockdown phases except for phase 3. Interestingly, the time of daily maximum was observed to be delayed by ~ 2 h over Delhi (from 1300 to 1500 h) and ~ 1 h over Kolkata (from 1300 to 1400 h) almost coinciding with the time of maximum temperature, highlighting the role of meteorology versus precursors. Emission reductions weakened the chemical sink of O
3
leading to enhancement (120%; 11 ppbv) in night-time O
3
over Delhi during phases 1–3.
Supplementary Information
The online version contains supplementary material available at 10.1007/s11356-021-16874-z.