We investigated variations of PM2.5and water-soluble inorganic ions chemical characteristics at nine urban and rural sites in China using ground-based observations. From 2015 to 2019, mean PM2.5concentration across all sites decreased by 41.9 μg/m~3with a decline of 46%at urban sites and 28% at rural sites, where secondary inorganic aerosol （SIAs） contributed to 21% （urban sites） and 17% （rural sites） of the decreased PM2.5. SIAs concentrations underwent a decline at urban locations, while sulfate (SO42–), nitrate （NO3–）, and ammonium（NH4+） decreased by 49.5%, 31.3% and 31.6%, respectively. However, only SO42–decreased at rural sites, NO3–increased by 21% and NH4+decreased slightly. Those changes contributed to an overall SIAs increase in 2019. Higher molar ratios of NO3–to SO42–and NH4+to SO42–were observed at urban sites than rural sites, being highest in the heavily polluted days.Mean molar ratios of NH3/NHxwere higher in 2019 than 2015 at both urban and rural sites,implying increasing NHxremained as free NH3. Our observations indicated a slower transition from sulfate-driven to nitrate-driven aerosol pollution and less efficient control of NOx than SO2related aerosol formation in rural regions than urban regions. Moreover, the common factor at urban and rural sites appears to be a combination of lower SO42–levels and an increasing fraction of NO3–to PM2.5under NH4+-rich conditions. Our findings imply that synchronous reduction in NOxand NH3emissions especially rural areas would be effective to mitigate NO3–-driven aerosol pollution.