Hybrid coating based on hyper-branched polyurethane and elemental sulfur was synthesized by in-situ polycondensation and urethane reaction. The effect of Sulfur in the hydrogen bonding, thermo-mechanical properties and surface morphology of HBPU-Urea-Sulfur hybrid coating at 2wt. % concentration was the notable objective of this work. Deconvolution studies confirmed that more hydrogen bonding interaction happened in HBPU-Urea coating, thereby shifting the characteristic peak position of N−H and C=O groups to lower wavenumber values. HBPU-Urea coating exhibited superior mechanical properties compared to HBPU-Urea-Sulfur hybrid coating. With the incorporation of 2 wt. % sulfur, the resultant hybrid coating showed decreasing in tensile strength and young’s modulus. Interestingly, the elongation at break percentage increased from 12% for HBPU-Urea to 18% for HBPU-Urea-Sulfur hybrid coating. Thermal stability of the coatings was examined by thermogravimetric analysis (TGA) depicted a 10°C decrease in thermal stability for 2 wt.% sulfur filled hybrid coating. DMTA measurements showed that the addition of sulfur nanoparticles decreased the glass transition temperature and crosslinking density. The HBPU-Urea-Sulfur hybrid coating displays a smooth surface because the size of the sulfur nanoparticles is reduced, leading to uniform dispersion and achieve good compatibility.