This chapter provides a conceptual overview of basic multicomponent self‐assembly principles and related problems of helicates. It explains the physico‐chemical concepts of fundamental processes dealing with the formation of metal‐ligand bonds and their supramolecular counterparts for mononuclear coordination compounds. These principles are then transposed to supramolecular helicates, highlighting the specific features accompanying this extension, especially the consideration of intramolecular interactions. Then, the chapter focuses on the description and assessment of cooperative interactions that play an important role in the stabilization of self‐assembled edifices. Kinetic factors are discussed in relation to the self‐assembly mechanisms of dinuclear helicates. The chapter also presents an overview of tools for assessing cooperativity in helicates. It describes the development and applications of thermodynamic modelling in detail. Finally, the chapter provides qualitative discussion on possible secondary interactions that control the structure of metallohelicates (helical conformational folding). Tutorial examples of helical assemblies are given across the whole chapter.