Following the first morphological and taxonomic inventory of Portuguese wheat in 1933, an archival collection of representative varieties has been maintained, replanted and documented by the National Institute of Agricultural and Veterinary Research (INIAV), specifically by its division formerly known as the National Station for Plant Improvement (ENMP-Elvas, now INIAV-Elvas). The INIAV-Elvas wheat collection has always been an invaluable asset in studies of agronomic and/or genetic development of wheat lines, as well as providing a frame of reference for the nutritional evolution of Portuguese wheat crops. This work addresses the status of selenium (Se) in a pool of 46 accessions of bread wheat. Special attention is paid to the (low) levels of Se, for which wheat acts as an important source in human diets, with a view to curbing its deficiency in Portuguese cultivars through biofortification strategies. All grain samples were irradiated at the Portuguese Research Reactor, and total Se was determined through cyclic neutron activation analysis. Our results indicate that the best candidates for an improvement of Se contents in mature grains are cvv. Ideal, Ribeiro (b) and Ribeiro (a), and the worst candidates are cvv. Restauração, Galego Rapado and Rieti.