For Pd-based catalysts, facile and fast interconversion between Pd and PdO occurs continuously during the CH 4 oxidation reaction, which makes it challenging to determine active sites. Herein, we report that the amount of partially oxidized palladium (PdO x ) on the catalyst surface shows a linear correlation with the CH 4 oxidation activity in a series of Pd/Al 2 O 3 and Pt− Pd/Al 2 O 3 catalysts hydrothermally aged under commercially relevant conditions. We characterized the amount of surface PdO x through diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) using CO as a probe molecule. With careful consideration that the redox cycle of Pd particles occurs continuously during the CH 4 oxidation reaction, the Pd/Al 2 O 3 catalysts were reoxidized before obtaining the CO adsorption DRIFTS data to minimize the discrepancy between the catalytically relevant phases and the characterized surface composition. The IR spectra of CO adsorption on reoxidized Pd/Al 2 O 3 catalysts contain peaks at 2135−2145 cm −1 , which correspond to PdO x . The steady-state CH 4 oxidation activities at 300 °C increased proportionally with the normalized surface PdO x . Furthermore, Pt−Pd bimetallic catalysts also showed the same linear correlation between the surface PdO x and CH 4 oxidation activity irrespective of composition, preparation method, and support. Our results indicate that the surface PdO x plays a critical role in determining CH 4 oxidation activity rather than the electronic properties of Pd. Overall, we report a general correlation between the amount of surface PdO x and the steady-state CH 4 oxidation activities in various Pd-based catalysts. This work will greatly help in achieving the fundamental understanding of the CH 4 oxidation reaction on the PdO x surface and the further development of Pd-based catalysts for CH 4 oxidation with better activity.