Systems and methods for detecting clandestine fissile or radioactive material on the basis of emitted radiation and particles (such as neutrons and alpha particles) arising from within the material. Emission by the fissile or radioactive material is detected in conjunction with a conventional x-ray imaging system that includes an external source of illuminating penetrating radiation, at least one detector configured to detect at least the penetrating radiation and to generate a detector signal, and a processor configured as a detector signal discriminator to generate an output indicating whether the detector signal is triggered by an origin other than illuminating penetrating radiation. Active and passive modes of detection are described by some embodiments. Other embodiments are directed toward neutron detection, gamma ray detection with energy resolution, and designs of detectors to enhance the detection of clandestine nuclear material.