Brazil is one of the world’s largest beer producers and also a major food producer. These activities generate a large amount of residues which, if disposed of inappropriately, can have adverse effects on the environment. The objective of this research was to evaluate the potential of using these residues for both mushroom cultivation (traditional use) and the production of mycelium-based composites (innovative use). Mushroom production (Pleurotus sajor-caju) was conducted using only brewer’s spent grains (fresh and dried) and also mixed with banana leaves (1:1) or peach palm leaves (1:1), which are residues widely available in the northern region of Santa Catarina, Brazil. The productivity of mushrooms cultivated using fresh and dried brewer’s spent grains did not exhibit a statistically significant difference, indicating that this residue can be utilized shortly after its generation in the industrial process, thereby reducing costs associated with production. Combining brewer’s spent grains with banana or peach palm leaves resulted in enhanced mushroom production (0.41 and 0.38 g day−1, respectively) compared to using the leaves as a sole substrate. The mushrooms produced contain sugars and a minimal sodium content, and are considered a source of phosphorus. In addition, no toxic elements (Hg and Pb) were present. The mycelium-based composites produced using the residual substrate (after the mushroom harvest) exhibited better mechanical properties (compressive strength = 0.04 MPa, density = 242 kg m−3, and low humidity sorption) than those produced using fresh substrate. The results demonstrate the synergistic effect of combining the two approaches under investigation. The use of brewer´s spent enhance the mushroom productivity and the residual substrate enhance the mechanical properties of mycelium-based composites. The compressive strength, density, and air humidity sorption properties are essential for determining the potential applications of mycelium-based composites. The use of brewer’s spent grains mixed with banana leaves demonstrated significant promise for mushroom production and subsequent application in the development of mycelium-based composites. These sequential approaches contribute to waste valorization and the rational utilization of natural resources, as the mycelium-based composites are considered for substitution of synthetic materials, thereby promoting sustainability for future generations.