It is crucial to accurately describe the interaction between the surface functionality and the supported metal catalyst because it directly determines the activity and selectivity of a catalytic reaction. It is, however, challenging with a metal-carbon catalytic system owing to the ultrafine feature, instability, and subtle response of the components upon application of an external field. Herein, we use insitu TEM, electron energy loss spectroscopy, and X-ray photoelectron spectroscopy techniques to record the interaction in palladium on carbon nanotubes (CNTs) from room temperature to 600 degrees C. We focus on probing the effects of oxygen and nitrogen-containing functional groups on supported palladium nanoparticles (NPs) in the model catalytic system. The stability of palladium NPs supported on CNTs depends strongly on the surface properties of CNTs. Moreover, the oxygen-containing functional groups on the CNT surfaces, such as carboxylic acids and anhydrides, have an even stronger interaction with palladium NPs than the nitrogen-containing counterparts. Our work contributes to elucidation of the complex metal-carbon interaction and unlocks potential in activity and selectivity control of these catalytic systems.