Solid oxide fuel cells (SOFCs) have potential to be the most efficient and cost-effective system for direct conversion of a wide variety of fuels to electricity. The performance and durability of SOFCs depend strongly on the microstructure and morphology of cell components. As a unique synthesis and processing technique with easy control of composition, structure, morphology, and microstructure, sol-gel processes have been widely used for fabrication of key SOFC materials or critical components with desired properties or functionalities unattainable otherwise. In this chapter, we provide an overview on sol-gel processes applied for preparation of homogeneous and fine powders of electrolyte, electrode, and ceramic interconnect materials, for deposition of dense electrolyte membranes or porous electrode films, and for modification of electrode or metallic interconnect surface or interface to enhance catalytic activity, to improve tolerance to coking or contaminant poisoning, and to increase stability against oxidation, reduction, or other degradation mechanisms. While significant progress has been made in controlling and tailoring the composition, microstructure, morphology, and hence functionality of materials and components, many challenges still remain to make sol-gel processes cost-effective and versatile for many applications. The development of novel sol-gel processes as well as the exploration of the existing ones to new applications continues to be an intriguing research pursuit.