Abnormal increases in radon ((222)Rn, half-life = 3.82 days) activity have occasionally been observed in underground environments before major earthquakes. However, (222)Rn alone could not be used to forecast earthquakes since it can also be increased due to diffusive inputs over its lifetime. Here, we show that a very short-lived isotope, thoron ((220)Rn, half-life = 55.6 s; mean life = 80 s), in a cave can record earthquake signals without interference from other environmental effects. We monitored (220)Rn together with (222)Rn in air of a limestone-cave in Korea for one year. Unusually large (220)Rn peaks were observed only in February 2011, preceding the 2011 M9.0 Tohoku-Oki Earthquake, Japan, while large (222)Rn peaks were observed in both February 2011 and the summer. Based on our analyses, we suggest that the anomalous peaks of (222)Rn and (220)Rn activities observed in February were precursory signals related to the Tohoku-Oki Earthquake. Thus, the (220)Rn-(222)Rn combined isotope pair method can present new opportunities for earthquake forecasting if the technique is extensively employed in earthquake monitoring networks around the world.