Bitter vetch (Vicia ervilia Willd.) is a traditional Mediterranean-West Asian legume, mainly used as livestock feed because of its toxic non-proteinogenic amino acid, canavanine. However, historical sources suggest its past human consumption. Currently, bitter vetch is a minor crop confined to marginal soils in semi-arid regions, presenting a potential alternative protein source amid projected climate changes. This study evaluated the nutritional and sensory attributes of bitter vetch seeds processed through various household methods. Germination and cooking significantly reduced the canavanine content by 28% and 60%, respectively. Incorporating bitter vetch flour (BVF) into wheat bread enhanced protein and fiber contents without substantially altering carbohydrate and lipid levels, and the baking process reduced the canavanine content by 40%. Bitter vetch flour enriched the bread with iron and calcium, contributing significantly to their daily nutritional intakes. Sensory evaluations indicated positive reception for bread with 12% BVF, achieving a balance between nutritional enhancement and consumer acceptance. This study identifies bitter vetch seeds as a valuable resource for improving bread formulations with corrected gluten contents and enhanced protein quality, as measured using protein-digestibility-corrected amino acid score (PDCAAS) values. With strategic processing and formulation adjustments, bitter vetch has the potential to re-emerge as a feasible high-protein grain crop, promoting sustainable farming.