Group-III nitrides, touted as the next-generation semiconductors beyond Si, have brought dramatic changes to our everyday life over the past 3 decades. With revolutionary applications in LED lighting and power electronics, the use of III-nitride semiconductors as catalysts for chemical reactions has also attracted extensive interests. However, while inorganic reactions, such as water-splitting, CO₂ reduction, and N₂ fixation, have made impressive achievements, the use of III-nitrides as organic reaction catalysts has received much less attention. In this review, we summarize the use of III-nitrides in the activation of covalent bonds in organic molecules to achieve more efficient or greener reactivity. With both thermal-driven and photo-driven reactions covered for a wide range of substrates, this review could inspire more innovations in the exploration of catalysis using “the semiconductors of the future,” while at the same time help bridge the boundaries of electronics and chemistry, sparking more interdisciplinary collaborations.