There exists an ongoing need to develop and improve methods of detecting radioactive materials. Since each radioactive isotope leaves a unique mark in a form of the particles it emits, new materials capable of detecting and measuring these particles are constantly sought. Neutrons and their detectors play a significant role in areas such as nuclear power generation, nuclear decommissioning and decontamination, border security, nuclear proliferation and nuclear medicine. Owing to the complexity of their detection, as well as scarcity of 3He, which has historically been the preferred choice for neutron detection in many application fields, new sensitive materials are sought. Organic and inorganic scintillating crystals have been recognised as particularly good alternatives and as such systems that utilise them are increasingly common. Since they allow investigation of the neutron energy spectra, greater information about the radioactive source can be inferred. Therefore, in this article an extensive review of scintillating crystals used for neutron detection is presented. By describing the history of scintillating crystals and discussing changes that occurred in their use and development of methods for radiation detection, the authors present a comprehensive overview of the current situation. Supported by a practical example, possible future directions of the research area are also presented.