Zinc (Zn) deficiency represents a significant global concern, affecting both plant and human health, particularly in regions with Zn-depleted soils. Agronomic biofortification strategies, such as the application of Zn fertilizers, offer a cost-effective approach to increase Zn levels in crops. This study aimed to assess the efficacy of soil and foliar Zn biofortification, applied as an aqueous solution of 0.5% zinc sulphate (ZnSO4·7H2O), on triticale (x Triticosecale) grown under Mediterranean conditions. The study was conducted over two growing seasons (2017/18 and 2018/19) in southern Spain, evaluating the effects on biomass yield; forage quality, including crude protein, Van Soest detergent fiber, organic matter digestibility, and relative forage value; and nutrient accumulation. Soil treatment consisted in the application of 50 kg of ZnSO4·7H2O ha-1 solely at the beginning of the first campaign to assess the residual effect on the second year. In contrast, the foliar treatment consisted of two applications of 4 kg of ZnSO4·7H2O ha-1 per campaign, one at the beginning of tillering and the other at the appearance of the first node. The foliar application increased the Zn content of the forage to adequate levels, while the soil application resulted in a 33% increase in biomass production, which is particularly beneficial for farmers. Overall quality was favored by the combined soil + foliar application, and no adverse antagonistic effects on other nutrients were detected. Instead, a synergistic interaction between Se and Zn was observed, which improved the efficacy of this important micronutrient for livestock and human wellbeing.