Nitrate aerosol makes up a significant fraction of fine particles and plays a key role in regional air quality and climate. The North China Plain (NCP) is one of the most industrialized and polluted regions in China. To obtain a holistic understanding of the nitrate pollution and its formation mechanisms over the NCP region, intensive field observations were conducted at three sites during summertime in 2014–2015. The measurement sites include an urban site in downtown Jinan – the capital city of Shandong Province –, a rural site downwind of Jinan city, and a remote mountain site at Mt. Tai (1534 m a.s.l.). Elevated nitrate concentrations were observed at all three sites despite distinct temporal and spatial variations. Using historical observations, the nitrate ∕ PM 2.5 and nitrate ∕ sulfate ratios have statistically significantly increased in Jinan (2005–2015) and at Mt. Tai (from 2007 to 2014), indicating the worsening situation of regional nitrate pollution. A multiphase chemical box model (RACM–CAPRAM) was deployed and constrained by observations to elucidate the nitrate formation mechanisms. The principal formation route is the partitioning of gaseous HNO 3 to the aerosol phase during the day, whilst the nocturnal nitrate formation is dominated by the heterogeneous hydrolysis of N 2 O 5 . The daytime nitrate production in the NCP region is mainly limited by the availability of NO 2 and to a lesser extent by O 3 and NH 3 . In comparison, the nighttime formation is controlled by both NO 2 and O 3 . The presence of NH 3 contributes to the formation of nitrate aerosol during the day, while there is slightly decreasing nitrate formation at night. Our analyses suggest that controlling NO x and O 3 is an efficient way, at the moment, to mitigate nitrate pollution in the NCP region, where NH 3 is usually in excess in summer. This study provides observational evidence of a rising trend of nitrate aerosol as well as scientific support for formulating effective control strategies for regional haze in China.