We used the GEOS-Chem model and its adjoint to quantify Chinese non-methane volatile organic compound (NMVOC) emissions for the year 2007, using the vertical column concentrations of formaldehyde and glyoxal observed by the Global Ozone Monitoring Experiment-2A (GOME-2A) instrument and the Ozone Monitoring Instrument (OMI) as constraints. We conducted a series of inversion experiments using different combinations of satellite observations to explore the impacts on top-down emission estimates due to different satellite retrievals. Our top-down estimates for Chinese annual total NMVOC emission was 23.4 to 35.4 (average 30.8) Tg C y<sup>−1</sup>, including 13.5 to 19.7 (average 17.0) Tg C y<sup>−1</sup> from anthropogenic sources, 8.9 to 14.8 (average 12.6) Tg C y<sup>−1</sup> from biogenic sources, and 1.1 to 1.5 (average 1.2) Tg C y<sup>−1</sup> from biomass burning. In comparison, the most widely-used bottom-up estimate for Chinese annual total NMVOC emission was 27.4 Tg C y<sup>−1</sup>, including 15.5 Tg C y<sup>−1</sup> from anthropogenic sources, 10.8 Tg C y<sup>−1</sup> from biogenic sources, and 1.1 Tg C y<sup>−1</sup> from biomass burning. The simultaneous use of glyoxal and formaldehyde observations helped distinguish the NMVOC species from different sources and was essential in constraining anthropogenic emissions. Our four inversions consistently showed that the emissions of Chinese anthropogenic NMVOC precursors of glyoxal were larger than the <i>a priori</i> estimates. Our top-down estimates for the Chinese annual emission of anthropogenic aromatics (benzene, toluene, and xylene) ranged from 5.0 to 7.3 Tg C y<sup>−1</sup>, 2 % to 49 % larger than the estimate of the bottom-up inventory (4.9 Tg C y<sup>−1</sup>). Model simulations using the average of our top-down NMVOC emission estimates showed that surface afternoon ozone concentrations over northern and central China increased 5–12 ppb in June and decreased 5–13 ppb in December relative to the simulations using the <i>a priori</i> emissions and were in better agreement with measurements. We concluded that the satellite observations of glyoxal and formaldehyde together provided quantitative constraints on the emissions and source types of NMVOCs over China and improved our understanding on regional chemistry.