The nanostructured boron composites generally have large amounts of boron contents and thus have the potential to deliver significant amount of boron to the tumor cells, that is crucial for boron neutron capture therapy (BNCT). In theory, BNCT is based on a nuclear capture reaction with the 10B isotope absorbing a slow neutron to initiate a nuclear fission reaction with the release of energetic particles, such as lithium and helium (α particles), which travel the distance of around nine microns within the cell DNA or RNA to destroy it. The recent studies have demonstrated that the nanostructured boron composites can be combined with the advanced targeted drug delivery system and drug detection technology. The successful combination of these three areas should significantly improve the BNCT in cancer treatment. This review summarizes the latest developments in this unique area of cancer therapy.