Ru/TiO 2 catalysts exhibit an exceptionally high activity in the selective methanation of CO in CO 2 -and H 2 -rich reformates,b ut suffer from continuous deactivation during reaction. This limitation can be overcome through the fabrication of highly active and non-deactivating Ru/TiO 2 catalysts by engineering the morphology of the TiO 2 support. Using anatase TiO 2 nanocrystals with mainly {001}, {100}, or {101} facets exposed, we show that after an initial activation period Ru/TiO 2 -{100} and Ru/TiO 2 -{101} are very stable,w hile Ru/ TiO 2 -{001} deactivates continuously.E mploying different operando/in situ spectroscopies and ex situ characterizations, we show that differences in the catalytic stability are related to differences in the metal-support interactions (MSIs). The stronger MSIs on the defect-richT iO 2 -{100} and TiO 2 -{101} supports stabilize flat Ru nanoparticles,w hile on TiO 2 -{001} hemispherical particles develop.The former MSIs also lead to electronic modifications of Ru surface atoms,r eflected by the stronger bonding of adsorbed CO on those catalysts than on Ru/TiO 2 -{001}.