Accurate measurements of methane (CH4) emissions from feedlot cattle are required for verifying greenhouse gas (GHG) accounting and mitigation strategies. We investigate a new method for estimating CH4 emissions by examining the correlation between CH4 and carbon dioxide (CO2) concentrations from two beef cattle feedlots in Australia representing southern temperate and northern subtropical locations. Concentrations of CH4 and CO2 were measured at the two feedlots during summer and winter, using open-path Fourier transform infrared spectroscopy. There was a strong correlation for the concentrations above background of CH4 and CO2 with concentration ratios of 0.008 to 0.044 ppm/ppm (R2 >0.90). The CH4/CO2 concentration ratio varied with animal diet and ambient temperature. The CH4/CO2 concentration ratio provides an alternative method to estimate CH4 emissions from feedlots when combined with CO2 production derived from metabolisable energy or heat production.