In this study, the integration of paper industry waste with high cellulose content into biocomposites of polylactic acid (PLA), a widely used biobased polymer material, was investigated. The PLA/waste biocomposite samples (0–25 wt.%) were manufactured using the extrusion and injection moulding techniques. The mechanical test results showed improvements in terms of tensile properties and a decrease in impact strength as the percentage of residue increased. The melting temperature decreased, and the crystallinity increased in all biocomposites according to the Differential Scanning Calorimetry (DSC) analysis. Water absorption increased proportionally with the percentage of residue, attributed to the higher cellulose content in the biocomposites, determined by Fourier transform infrared spectroscopy (FT-IR) and X-ray diffraction (XRD) techniques. The scanning electron microscopy (SEM) fracture analysis demonstrated effective reinforcement–matrix cohesion, supporting the previously observed behaviour of the analysed materials. This work highlights the potential of using waste from the paper industry as reinforcement in PLA matrices, opening new perspectives for sustainable applications in the framework of the manufacture of composite materials.