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CuFeO2 multiferroics were fabricated under high pressure and high temperature for the first time, and their microstructures and magnetic properties were investigated systematically. Compared with the conventional state-solid reaction method, high pressure was conducive to obtaining CuFeO2 ceramics with preferred orientation and dense morphology. Phase-pure CuFeO2 was obtainable with Cu2O and Fe2O3 as starting materials. Though all samples exhibited two successive magnetic transitions at low temperatures, the magnetic transition temperatures in high-pressure synthesized sample decreased compared to the sample as prepared under ambient pressure.