The essentiality of selenium (Se) and iodine (I) to human beings and the widespread areas of selenium and iodine deficiency determine the high significance of functional food production with high levels of these elements. In this respect, joint biofortification of agricultural crops with Se and I is especially attractive. Nevertheless, in practice this topic has raised many problems connected with the possible utilization of many Se and I chemical forms, different doses and biofortification methods, and the existence of wide species and varietal differences. The limited reports relevant to this subject and the multiplicity of unsolved questions urge the need for an adequate evaluation of the results obtained up-to-date, useful for developing further future investigations. The present review discusses the outcome of joint plant Se–I biofortification, as well as factors affecting Se and I accumulation in plants, paying special attention to unsolved issues. A particular focus has been given to the prospects of herb sprouts production enriched with Se and I, as well as the interactions between the latter microelements and arbuscular-mycorrhizal fungi (AMF).