Global concern for the illicit transportation and trafficking of nuclear materials and other radioactive sources is on the rise, with efficient and rapid security and non-proliferation technologies in more demand than ever. Many factors contribute to this issue, including the increasing number of terrorist cells, gaps in security networks, politically unstable states across the globe and the black-market trading of radioactive sources to unknown parties. The use of passive gamma-ray and neutron detection and imaging technologies in security-sensitive areas and ports has had more impact than most other techniques in detecting and deterring illicit transportation and trafficking of illegal radioactive materials. This work reviews and critically evaluates these techniques as currently utilised within national security and non-proliferation applications and proposes likely avenues of development.