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During the early phase of a nuclear accident, major radioactive materials are released into the environment, necessitating the prompt deployment of various protective actions to avoid or reduce radiation exposure. To implement these actions, the levels of radioactivity in the environment should be determined. However, the radioactivity concentrations of artificial alpha-particle-emitting radionuclides such as plutonium are difficult to measure in airborne samples, because they are interfered with natural radionuclides such as uranium decay products. Therefore, chemical separation is required to measure the concentrations. This study presents a new emergency monitoring system for airborne samples, which performs multiple-pulse time-interval analysis (MTA) without chemical separation. The system is used in conjunction with an alpha/beta-particle survey meter and adopted an analysis method focusing on the detected time interval of each particle. Its features are that a short time to output measurement result, easy handling and nondestructive. The estimated detection limit of the system was 9.5 × 10−2 Bq m−3. The MTA-based monitoring system could be useful in situations requiring prompt measurement and screening of samples.