This paper reports on the development of a method for enhanced non-destructive assay (NDA) of radioactive waste using the novel technique neutron-gamma emission tomography (NGET). The technique relies on the detection of correlated fast neutrons and gamma rays emitted in spontaneous or induced fission. It is based on fast organic scintillators and enables sensitive detection and three-dimensional (3D) localization of the fission events. The technique is passive and does not require moving components. In this work, we apply the NGET technique to the category of radioactive waste which is often referred to as historic or legacy waste. This can include mixed wastes encased in shielded containers many decades ago, before the advent of detailed waste description criteria. These low or intermediate level wastes are often associated with lacking, limited or conflicting documentation. This poses a challenge when assigning the waste to the proper disposal route as well as in deciding whether the waste needs to undergo sorting and conditioning to fulfil waste acceptance criteria both with regards to safe interim storage and to its ultimate disposal. Actinides, such as isotopes of uranium and plutonium, with their typically long half-lives and decay chains are of special interest in this regard since they may challenge the long-term safety assessment in repositories predicated on mainly shorter half-life radionuclides if undetected. Accurate identification and localisation of actinides is also important from a safeguards perspective, especially since they are generally difficult to detect and localise by established passive means due to their relatively weak radiation emissions, in particular in shielded containments and in the presence of strong radiation fields from other radioactive materials. In this paper we present findings of measurements on shielded containments of long-lived radioactive waste performed at the Studsvik site in Sweden, as well as measurements on a laboratory assembly simulating a grouted waste drum. Similarities and differences between the novel NGET technique and a commercially available gamma imaging system are also briefly discussed.