Cyclodextrins (CDs)—a class of water-soluble seminatural cyclic oligosaccharides—comprise α-D-glucopyranose units linked by 1,4-glycosidic linkages. It gained significant attention in the scientific community because of the potential applications in synthetic organic and material chemistry, attributed to its toroidal three-dimensional flexible structures, consisting of a narrow upper rim and a larger bottom rim. Due to several polar carbohydrate moieties, they do not absorb UV–Vis light; nevertheless, they can act as precursors for forming spectroscopically sensitive compounds through several modifications. Synthetic alterations to the cyclodextrin structure can significantly alter the steric layout, hydrophobicity, and charge density, possibly making the formation of host-guest complexes suitable for various applications more effective. This book chapter provides a collection of processes reported in recent literature about constructing cyclodextrins as versatile chemical sensors via molecular recognition phenomena for sensing ions and other small molecular species.