In this paper we present an ultrasonic pulseecho technique for estimating the methane (CH4) content in binary mixtures of CH4 and carbon dioxide (CO2). The method is based on parametric estimation of phase velocity and frequency dependent attenuation in combination with Partial Least-Squares Regression (PLSR). The technique is verified using experiments on mixtures with a volume fraction of CO2 in the range of 0 % -10 %. The experiments show that the CH4 content can be accurately estimated with high repeatability.