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Terrein is one of the most important biomolecules of fungal origin being studied from a medicinal perspective. Secondary metabolites are the intermediate products produced during the metabolism of organisms for a large number of functions, for example, defense and communication signals. From the outset, terrein has largely been studied as an anticancer secondary biomolecule. Aspergillus terreus is the only fungal source of some valuable drugs and mycotoxins. From the beginning, a few species of Aspergillus were known to be viable chemical factories. Terrein is a potent biological molecule present in the fungus that is responsible for its medicinal and agricultural values. Numerous evaluations conducted on terrein showed it to have marked biological activities (antimicrobial, antiproliferative, anti-oxidative, and others). To date, terrein has emerged as a very attractive therapeutic regimen against cancer due to its dual targeting nature; tumor angiogenesis and cell proliferation. This focused review provides details of the therapeutic value of terrein and its modes of action as an anticancer agent. Besides this, terrein has other marked bioactivities and manifold uses in the field of medicine, which have also been discussed here.