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In current scenario, heterocyclic compounds' role in medicinal chemistry has been tremendously increased as they possess wide number of pharmacological activities. One of the common heterocycles include indole skeleton with well‐established biological significance in field of medicinal chemistry. Fusion of indole nucleus with pyrrole heterocycle constitutes pyrroloindole scaffold, which further modifies the existing properties of indole alone. Pyrroloindole is a privileged scaffold found in various types of bioactive entities including natural compounds and exhibits wide variety of pharmacological activities like muscle relaxant, antifungal, antitumor, and antibiotic. Therefore, it is considered as attractive template for drug discovery. From several years, numbers of synthetic strategies have been reported for the synthesis of pyrroloindole and its derivatives, including also natural compounds such as amauromine …