The main objective of this experiment was to investigate the technological potential of upcycling unsparged non-conventional brewers’ spent grains (BSGs) in bread-making and assess the comparative quality of bread enriched with non-fermented and lactic acid-fermented BSGs obtained from mashes brewed with starch adjuncts of buckwheat and oats. After the runoff of the first wort, unsparged non-conventional BSGs with approximately 75% moisture, acidic pH, and yield in the soluble extract above 56.6% (w/w d.m.) were used in substituting wheat flour with 5 and 15% (w/w d.m.) in bread-making recipes. The highest loaf volume value (318.68 cm3/100 g) was observed for 5% fermented buckwheat-BSG addition. Except for the samples with 5% fermented BSGs, specific volumes decreased. Crumb moisture was reduced by up to 22% for all samples, with this parameter related to bread weight. Bread porosity, elasticity, acidity, and overall sensory acceptability were better for fermented than non-fermented BSGs. The results proved that non-conventional BSGs with buckwheat and oats addition have the potential to be valorized in new bread assortments, and lactic acid fermentation applied to the BSGs is beneficial, even for overall sensory acceptability and quality of baked end-products. Technological, buckwheat-BSG was more convenient than oats-BSG. Further research continues to optimize and upscale Technology Readiness Levels.