Municipal solid waste (MSW) landfills can generate significant amounts of methane. There is considerable interest in quantifying surface methane emissions at such facilities. Numerous techniques exist for the evaluation of methane emissions from landfills. These techniques are either based on analytical emission models or on measurement methods. This paper presents a method to estimate methane emissions using ambient air methane measurements obtained on the surface of a landfill. Genetic algorithms (GA) based optimization combined with the standard Gaussian dispersion model are employed to identify locations as well as emission rates of potential emission sources throughout a MSW landfill. A case study is employed to evaluate the performance of the proposed methodology. GA-based search techniques are proven to be useful in estimating source locations and emission rates using methane concentration measurements.