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The influence of the nature of carbon materials used as a support for Ru/C catalysts on levulinic acid hydrogenation with formic acid as a hydrogen source toward gamma-valerolactone was investigated. It has been shown that the physicochemical properties of carbon strongly affect the catalytic activity of Ru catalysts. The relationship between the hydrogen mobility, strength of hydrogen adsorption, and catalytic performance was established. The catalyst possessing the highest number of defects, stimulating metal support interaction, exhibited the highest activity. The effect of the catalyst grain size was also studied. It was shown that the decrease in the grain size resulted in the formation of smaller Ru crystallites on the catalyst surface, which facilitates the activity.