Methane (CH 4 ) and carbon monoxide (CO) mixing ratios were measured at an air quality monitoring station near the Mt. Wilson (MW) Observatory in southern California starting in the spring of 2007. Diurnal variation and mixing ratio correlation (R 2 = 0.81) were observed. The correlation results observed agree with previous aircraft measurements collected over the greater Los Angeles (LA) metropolitan area. The consistent agreement between CH 4 and CO indicates these gases are well-mixed before reaching the sampling site and the emission source contributions of both compounds are reasonably constant. Since CH 4 and CO are considered non-reactive on the time scale of dispersion within the LA urban area and their emission sources are likely to be similarly distributed (e.g., associated with human activities) they are subject to similar scales of atmospheric transport and dilution. This behavior allows the relationship of CH 4 and CO to be applied for estimation of CH 4 emissions using well-documented CO emissions. Applying this relationship a “top–down” CH 4 inventory was calculated for LA County based on the measurements observed at MW and compared with the California Air Resources Board (CARB) “bottom–up” CH 4 emissions inventory based on the Intergovernmental Panel on Climate Change recommended methodologies. The “top–down” CH 4 emissions inventory is approximately one-third greater than CARB's “bottom–up” inventory for LA County. Considering the uncertainties in both methodologies, the different CH 4 emissions inventory approaches are in good agreement, although some under and/or uninventoried CH 4 sources may exist.