Nitriles are a versatile family of nitrogen-containing organic compounds widely used in the fields of analytical, synthetic, medicinal, and polymer chemistry. Among the numerous synthetic routes, the conversion of primary alcohols into nitriles is particularly noteworthy due to its benefits of a good atom economy, a diversified substrate scope, concise reaction pathways, and satisfactory catalytic efficiency. Herein, the research progress in the methodologies for converting primary alcohols into nitriles is summarized, including conventional thermal homogeneous catalysis and heterogeneous (ammonoxidation and dehydroamination) catalysis as well as emerging photocatalysis and electrocatalysis. The catalyst systems, reaction mechanisms, substrate compatibility, and current limitations of the different routes are highlighted. Finally, future perspectives of nitrile production on a largescale are proposed from the viewpoints of route characteristics, technological maturity, and fundamental research directions.