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Scaffolds supplemented with naturally derived materials seem to be a good choice in bone tissue engineering. This study aims to develop polyurethane (PU) nanofibers added with ylang ylang (YY) and zinc nitrate (ZnNO₃) using the electrospinning method. Field emission scanning electron microscopy (FESEM) images showed that the diameter of the PU nanofibers (869 ± 122 nm) was reduced with the addition of YY and ZnNO₃ (PU/YY—467 ± 132 nm and PU/YY/ZnNO₃—290 ± 163 nm). Fourier transform infrared (FTIR), a thermal gravimetric analysis (TGA) and an X-ray diffraction (XRD) analysis confirmed the interactions between PU with YY and ZnNO₃. In addition, a thermal gravimetric analysis (TGA) study revealed the improved thermal stability for PU/YY and a slight reduction in the thermal stability for PU/YY/ZnNO₃. A tensile test indicated that the addition of YY and ZnNO3 (PU/YY—12.32 MPa and PU/YY/ZnNO₃—14.90 MPa) improved the mechanical properties of the pristine PU (6.83 MPa). The electrospun PU/YY (524 nm) and PU/YY/ZnNO₃ (284 nm) showed a reduced surface roughness when compared with the pristine PU (776 nm) as depicted in the atomic force microscopy (AFM) analysis. The addition of YY and ZnNO₃ improved the anticoagulant and biocompatibility nature of the pristine PU. Furthermore, the bone mineralization study depicted the improved calcium deposition in the fabricated composites (PU/YY—7.919% and PU/YY/ZnNO₃—10.150%) compared to the pristine PU (5.323%). Hence, the developed composites with desirable physico-chemical properties, biocompatibility and calcium deposition can serve as plausible candidates for bone tissue engineering.