The wide use of natural fibers has a long-standing history in Africa. In northern Angola, three native fiber plant species, namely Urena lobata, Triumfetta cordifolia, and Dombeya burgessiae, were investigated with regard to their potential usage in modern applications, such as green composites. Bast fibers of the three species were analyzed morphologically, chemically, and mechanically to determine properties such as fiber density, cellulose content, Young’s modulus, tensile strength, and breaking strain. In comparison to other natural fibers, all three species were characterized by high Young’s moduli up to 60 GPa and tensile strengths up to 950 MPa, yet retting is crucial to unfold the maximum strength of the fibers. Extending the retting time revealed higher values but probably negatively influences economic efficiency. The results demonstrated that the analyzed plants deliver strong and resistant fibers; based on their biomechanical performance, they are alternatives to commercially used natural fibers, such as jute (Corchorus spp.). However, as with other natural fibers, there was high variation in the mechanical properties in the studied species.