Selenium (Se) and zinc (Zn) deficiencies affect up to 15% and 17% of the global population, respectively. Agronomic biofortification of staple crops with Se/Zn may alleviate these challenges. Pea (Pisum sativum L.) is a nutritious legume crop with great potential for Se/Zn biofortification. Herein, two varieties of pea (Ambassador, Premium) were biofortified via foliar application of sodium selenate (0/50/100 g of Se/ha) or zinc oxide (0/375/750 g of Zn/ha) during the flowering stage under field conditions. While no significant differences were found in Se accumulation between seed varieties upon Se treatments, selenate enhanced the accumulation of Se in the two seed varieties dose dependently. Selenium concentration was most elevated in seeds of Ambassador exposed to 100 g of Se/ha (3.93 mg/kg DW vs. the control (0.08 mg/kg DW), p < 0.001). 375 g of Zn/ha (35.7 mg/kg DW) and 750 g of Zn/ha (35.5 mg/kg DW) significantly and similarly enhanced Zn concentrations compared to the control (31.3 mg/kg DW) in Premium seeds, p < 0.001. Zinc oxide also improved accumulations of Fe, Cu, Mn, and Mg in Premium seeds. Se/Zn treatments did not significantly affect growth parameters and accumulations of soluble solids and protein in seeds. Consuming 33 g/day of pea biofortified with Se at 50 g/ha and 266 g/day of pea biofortified with 375 g of Zn/ha could provide 100% of the RDA for Se (55 µg) and Zn (9.5 mg) in adults, respectively. These results are relevant for enhancing Se/Zn status in peas by foliar biofortification.