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<i>Cirsium setidens</i> Nakai is a perennial plant extensively used as food in Korea. Various reports have illustrated the presence of phytochemicals with antioxidant, anti-cancer, anti-tumor, and anti-inflammatory activities; however, little is known about the volatile compounds present in this plant. Here, a novel solid-phase microextraction (SPME) Arrow method was performed to extract and analyze volatile compounds from freeze-dried <i>Cirsium setidens</i> Nakai. Four types of SPME Arrows coated with films, such as carbon wide range/polydimethylsiloxane, divinylbenzene/polydimethylsiloxane, polydimethylsiloxane, and polyacrylate were evaluated to identify the most suitable Arrow. The carbon wide range/polydimethylsiloxane Arrow was found to exhibit high affinity for the volatile compounds present in <i>Cirsium setidens</i> Nakai. A total of 58 volatile compounds were identified. The major compounds were 2-Pentylfuran, 1-Methylcycloheptanol, 1-Penten-3-ol, 2,2,4,6,6-Pentamethylheptane, 2,3,6,7-Tetramethyloctane, 5-Ethyl-2,2,3-trimethylheptane, 3,5-Octadien-2-one, β-Cyclocitral, and trans-β-Ionone. The present study demonstrates that the SPME Arrow coated with the carbon wide range/polydimethylsiloxane film is suitable for the analytical profiling of volatile compounds present in <i>Cirsium setidens</i> Nakai.