There remains significant uncertainty in the estimation of anthropogenic CH 4 emissions at local and regional scales. We used atmospheric CH 4 and CO 2 concentration data to constrain the anthropogenic CH 4 emission in the Yangtze River Delta one of the most populated and economically important regions in China. The observation of atmospheric CH 4 and CO 2 concentration was carried out from May 2012 to April 2017 at a rural site. A tracer correlation method was used to estimate the anthropogenic CH 4 emission in this region, and compared this "top-down" estimate with that obtained with the IPCC inventory method. The annual growth rates of the atmospheric CO 2 and CH 4 mole fractions are 2.5 ± 0.7 ppm year −1 and 9.5 ± 4.7 ppb year −1 , respectively, which are 9% and 53% higher than the values obtained at Waliguan (WLG) station. The average annual anthropogenic CH 4 emission is 4.37 (± 0.61) × 10 9 kg in the YRD (excluding rice cultivation). This "top-down" estimate is 20-70% greater than the estimate based on the IPCC method. We suggest that possible sources for the discrepancy include low biases in the IPCC calculation of emission from landfills, ruminants and the transport sector.Atmosphere 2019, 10, 185 2 of 21 activities and sums up the individual components to the domain of interest. One problem is that activity data, such as landfill and livestock, and emission factors cannot be accurately determined at the regional and the city scale [8][9][10]. A study in Beijing found that the uncertainty caused by landfill accounts for nearly half of the total uncertainty in the CH 4 emission estimate [11]. Accurate and timely calculations of anthropogenic CH 4 emissions at the regional scale are necessary for assessing the effectiveness of emission reduction policies.Anthropogenic greenhouse gas emissions can also be estimated from observations of the gaseous concentrations in the atmosphere ("top-down" methods). The "atmospheric method" used in this study is one of the "top-down" approaches. One reason for using the atmospheric method is that many sources of anthropogenic CH 4 cannot be quantified with traditional methods, such as the chamber method [12][13][14]. The atmospheric method requires simultaneous concentration measurements of the target gas (CH 4 ) and a tracer gas (usually CO 2 ) when there is no disturbance from sinks or other natural sources [15]. In an observational study using aircraft profile measurement over a broad region of Alaska and Canada, the concentrations of CH 4 and CO 2 increase synchronously with height, showing a strong positive correlation between the two gases [16]. A similar positive relationship also exists in the surface air in a moderately polluted urban atmosphere of Boulder, USA [16]. The explanation for the positive relationship is that the two gases share common source areas and undergo the same long-range transport [17,18]. The concentration ratio between the two gases were used to estimate the CH 4 emissions in the densely populated urban areas in Southern California, showing ...