Indoles are a significant heterocyclic system in natural products and drugs. They are important types of molecules and natural products and play a main role in cell biology. The application of indole derivatives as biologically active compounds for the treatment of cancer cells, microbes, and different types of disorders in the human body has attracted increasing attention in recent years. Indoles, both natural and synthetic, show various biologically vital properties. Owing to the importance of this significant ring system, the investigation of novel methods of synthesis have attracted the attention of the chemical community. In this review, we aim to highlight the construction of indoles as a moiety in selected alkaloids.