Faba bean (Vicia faba L.) has spread worldwide as an excellent source of proteins. To evaluate the efficiency of Se biofortification, four cultivars of V. faba (Belorussian, Russian Black, Hangdown Grünkernig, and Dreifach Weiβe) were foliar treated with 1.27 mM solutions of nano-Se, sodium selenate, and sodium selenite. Yield, protein, and Se contents were greatly affected by genetic factors and chemical form of Se. Selenium biofortification levels were negatively correlated with Se concentration in control plants and increased according to the following sequence: nano-Se < sodium selenite < sodium selenate. Contrary to selenate and selenite, nano-Se showed a growth-stimulating effect, improving yield, seed weight, and pod number. Pod thickness decreased significantly as a result of nano-Se supply and increased by 1.5–2.3 times under selenate and selenite supply. The highest Se concentrations were recorded in the seeds of Se-fortified cv. Belorussian and the lowest one in those of Se-treated Hangdown Grünkernig. Protein accumulation was varietal dependent and decreased upon 1.27 mM selenate and selenite treatment in the cvs. Hangdown Grünkernig and Dreifach Weiβe. The results indicate the high prospects of nano-Se supply for the production of faba bean seeds with high levels of Se.