This work investigated the addition of spent coffee grounds (SCG) as a valuable resource to produce biocomposites based on polylactic acid (PLA). PLA has a positive biodegradation effect but generates poor proprieties, depending on its molecular structure. The PLA and SCG (0, 10, 20 and 30 wt.%) were mixed via twin-screw extrusion and molded by compression to determine the effect of composition on several properties, including mechanical (impact strength), physical (density and porosity), thermal (crystallinity and transition temperature) and rheological (melt and solid state). The PLA crystallinity was found to increase after processing and filler addition (34–70% in the 1st heating) due to a heterogeneous nucleation effect, leading to composites with lower glass transition temperature (1–3 °C) and higher stiffness (~15%). Moreover, the composites had lower density (1.29, 1.24 and 1.16 g/cm3) and toughness (30.2, 26.8 and 19.2 J/m) as the filler content increased, which is associated with the presence of rigid particles and residual extractives from SCG. In the melt state, polymeric chain mobility was enhanced, and composites with a higher filler content became less viscous. Overall, the composite with 20 wt.% SCG provided the most balanced properties being similar to or better than neat PLA but at a lower cost. This composite could be applied not only to replace conventional PLA products, such as packaging and 3D printing, but also to other applications requiring lower density and higher stiffness.