Carbon formation within nickel-based solid oxide fuel cell (SOFC) anodes exposed to carbonaceous fuels typically leads to reduced operational lifetimes and performance, and can eventually lead to catastrophic failure through cracking and delamination. In-situ Raman spectroscopy has been shown to be a powerful characterization tool for the investigation of the dynamics of physical processes occurring within operational SOFCs in real time. Here we investigate the dynamics of carbon formation on a variety of nickel-based SOFC anodes as a function of temperature, fuel and electrical loading using Raman spectroscopy. We show that the rate of carbon formation throughout the SOFC anode can be significantly reduced through a careful consideration of the SOFC anode material, design and operational conditions. © The Electrochemical Society.