3D printing with biodegradable polymers such as polylactic acid (PLA) is a sustainable alternative to conventional petroleum-derived plastics. However, improving the mechanical properties of PLA remains a challenge. This study explores the incorporation of chemically treated hemp fibers to improve the interfacial adhesion and mechanical strength of PLA filaments. Samples with PLA and hemp were prepared by subjecting the fibers to cationization treatment with (3-chloro-hydroxypropyl) tri-methylammonium (EPTA) and functionalization with glycidyl methacrylate (GMA). EPTA improves adhesion mainly through surface modification, increasing reactive functional groups in cellulose, while GMA improves interfacial adhesion by forming covalent bonds with both the fiber and PLA and improves the dispersion of the fiber in the matrix. Mechanical properties were evaluated by tensile testing, as well as fracture morphology by scanning electron microscopy (SEM) and X-ray energy dispersive analysis (EDS). The results showed that the addition of untreated hemp significantly reduced the strength of PLA, but cationization with EPTA improved interfacial adhesion and increased tensile strength by 615%. The combination of treated fibers and GMA further optimized the mechanical properties, reaching values similar to pure PLA. These findings indicate that the chemical modification of natural fibers facilitates their integration into PLA filaments for 3D printing, promoting sustainable materials without compromising mechanical performance.