The quality of carbon anodes, consumed in electrolysis during the primary aluminum production, has an important impact on the electrolytic cell performance. Coke and pitch are the raw materials used in anode manufacturing. The raw material properties and the process parameters during production determine the anode quality. A plant receives these materials from different sources, and the variability in their properties is usually a major concern during anode production. The interaction between coke and pitch influences strongly the anode properties. Study of coke and pitch individually as well as the interactions between them (using different techniques (spectroscopic, optical, etc.) such as XRD, FTIR, XPS, SEM helps identify their compatibility. Each technique gives information on different aspects of the raw materials. In this article, the use of a number of these techniques for studying coke, pitch, and their interactions will be discussed. Results will be presented for a number of cases.