Despite the high value of ramson (Allium ursinum) in medicine and nutrition, it is not cultivated in open fields due to the need for shading as well as weeding during the early crop stages. Research was carried out in an open field with the aim to improve A. ursinum growth, through its intercropping with Armoracia rusticana (horseradish). In the latter context, with and without sodium selenate application, ramson and horseradish showed reciprocal growth stimulation, as ramson biomass increased by 1.28 times and horseradish root biomass by 1.7 times. The biofortification level of horseradish roots increased from 5.9 to 9.6 times due to joint plant growth under selenium (Se) supply. The opposite phenomenon was recorded for ramson leaves, as the biofortification level decreased from 11.7 in the case of Se supplementation to 6.7 in plants supplied with sodium selenate when jointly cultivated with horseradish. Among the tested antioxidants, the highest increase due to joint cultivation and/or Se supply was recorded for ascorbic acid by 1.69 times in ramson leaves and 1.48 and 1.37 times in horseradish roots and leaves, respectively. All treatments significantly increased the total antioxidant activity (AOA) of horseradish leaves (by 1.33–1.49 times) but not roots. Comparison of the results obtained in field conditions with those obtained earlier for the Se biofortification of ramson in the natural habitat (forest) revealed significantly higher levels of the plant’s antioxidant status under environmental stress (field) and a decrease in the correspondent differences as a consequence of Se biofortification. The estimation of allelopathic beneficial interaction between ramson and horseradish implies the efficiency of ramson growth and production of functional food with high levels of Se (Se–ramson leaves and Se–horseradish roots).