A novel UV-curable polyurethane acrylate (PUA) oligomer was synthesized by modifying cardanol with a polyfunctional acrylate precursor obtained through reacting pentaerythritol triacrylate with isophoronediisocyanate. Chemical structures of the obtained cardanol-based PUA (C-PUA) oligomer were confirmed by Fourier transform infrared and 1H NMR. Subsequently, viscosity and gel content of the C-PUA resins containing different quantities of hydroxymethyl methacrylate (HEMA) were characterized. The C-PUA oligomer possessed a viscosity of 8360 mPa s, which reduced to 115 mPa s when 40% of the HEMA diluent was added. Furthermore, thermal, mechanical, coating, and swelling properties of the resulting UV-cured C-PUA/HEMA materials were investigated. The ultimate biomaterials showed excellent performance, including a glass transition temperature (T g) of 74-123 °C, maximum thermal degradation temperature of 437-441 °C, tensile strength of 12.4-32.0 MPa, tensile modulus of 107.2-782.7 MPa, and coating adhesion of 1-2. In conclusion, the developed C-PUA resins show great potential to be applied in UV-curable materials like coatings.