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The biocontrol fungus <i>Trichoderma harzianum</i>, from both marine and terrestrial environments, has attracted considerable attention. <i>T. harzianum</i> has a tremendous potential to produce a variety of bioactive secondary metabolites (SMs), which are an important source of new herbicides and antibiotics. This review prioritizes the SMs of <i>T. harzianum</i> from 1988 to June 2022, and their relevant biological activities. Marine-derived SMs, especially terpenoids, polyketides, and macrolides compounds, occupy a significant proportion of natural products from <i>T. harzianum</i>, deserving more of our attention.