Increasing amounts of atmospheric CO2 has led to a recent resurgence in carbon capture processes for renewable energy storage. Production and storage of methane through CO2 and CO methanation have been widely accepted as the process by which carbon capture is performed. Widespread utilization of this process has been low, especially with CO2 methanation, as a result of the expensive nature of highly active catalysts and the low activity associated with inexpensive catalysts. Thus, developing a low-cost and highly active catalyst is desirable for widespread implementation. In past studies, nickel catalysts provided promising results in methanation processes, but because of its low catalytic activity, additional interest in enhancing nickel efficiency grew. The addition of manganese, another low-cost metal, to nickel promotes the overall activity of the catalyst. Unfortunately, information on how the bimetallic interactions enhance catalytic activity is scarce. Consequently, this study aims to shed light on the mechanistic processes of the Ni/Mn catalyst through extensive analytical analysis and computational modeling. Understanding the Ni/Mn synergism will be the focus of this presentation, including coverage of the crucial steps of the methanation mechanism that provide significant insight into the underlying processes leading to the enhanced activity of the bimetallic catalyst. One critical aspect of this work is the extensive analytical characterization performed on the Ni and Ni/Mn catalysts, including both bulk and analytical materials analyses.