ABSTRACT To propose a novel monitoring method for the quantitative visualization of 3D distribution of a radioactive plume in the vicinity of release point and source term estimation of released radionuclides, the feasibility of its analysis method is demonstrated by preliminary test. The proposed method is the combination of gamma-ray imaging spectroscopy with the electron tracking Compton camera (ETCC) and real-time high-resolution atmospheric dispersion simulation based on 3D wind observation with Doppler lidar. ETCC can acquire the angle distribution images of direct gamma-ray from a specific radionuclide in a target radioactive plume by quantitatively capturing gamma-ray incidence angles and spectrum distributions. The 3D distribution of each radionuclide in the radioactive plume is inversely reconstructed from direct gamma-ray images of each radionuclide by several ETCCs located around the target by harmonizing with the air concentration distribution pattern of the plume predicted by real-time atmospheric dispersion simulation. A prototype of the analysis method was developed, showing a sufficient performance in several test cases using hypothetical data generated by numerical simulations of atmospheric dispersion and radiation transport. The proposed method is expected to become an innovative monitoring framework for nuclear emergency.