The incorporation of fiber reinforcements into polymer matrices has emerged as an effective strategy to enhance the mechanical properties of composites. This study investigated the tensile and fracture behavior of 3D-printed polylactic acid (PLA) composites reinforced with chopped carbon fibers (CCFs) through experimental characterization and finite element analysis (FEA). Composite samples with varying CCF orientations (0°, 0°/90°, +45°/−45°, and 0°/+45°/−45°/90°) were fabricated via fused filament fabrication (FFF) and subjected to tensile and single-edge notched bend (SENB) tests. The experimental results revealed a significant improvement in tensile strength, elastic modulus, and fracture toughness compared to unreinforced PLA. The 0°/+45°/90° orientation exhibited a 3.6% increase in tensile strength, while the +45°/−45° orientation displayed a 29.9% enhancement in elastic modulus and a 29.9% improvement in fracture toughness (259.12 MPa) relative to neat PLA (199.34 MPa√m). An inverse correlation between tensile strength and fracture toughness was observed, attributed to mechanisms such as crack deflection, fiber bridging, and fiber pull-out facilitated by multi-directional fiber orientations. FEA simulations incorporating a transversely isotropic material model and the J-integral approach were conducted using Abaqus, accurately predicting fracture toughness trends with a maximum discrepancy of 8% compared to experimental data. Fractographic analysis elucidated the strengthening mechanisms, highlighting the potential of tailoring CCF orientation to optimize mechanical performance for structural applications.