In this study, the researchers successfully embellished the surface of halloysite (Ag/HNTs) with silver using halloysite, silver nitrate (AgNO3), and polyvinylpyrrolidone (PVP). The researchers then prepared polyurethane that contained pyridine ring by using 4,4′-diphenylmethane diisocyanate (MDI) and polytetramethylene glycol (PTMG) as the hard chain segment and the soft chain segment of polyurethane (PU), as well as 2,6-pyridinedimethanol (2,6-PDM) as the chain extension agent. This was followed by the preparation of Ag/HNTs/PUs nanocomposite thin films, achieved by mixing Ag/HNTs with different ratios into polyurethane that contains pyridine ring. First, the Ag/HNTs powders were analyzed using energy-dispersive X-ray spectroscopy, X-ray diffraction, and transmission electron microscopy. Subsequently, Fourier-transform infrared spectroscopy was used to examine the dispersibility of Ag/HNTs in PU, whereas the thermal stability and the viscoelasticity of Ag/HNTs/PU were examined using thermal gravimetric analysis, differential scanning calorimetry, and dynamic mechanical analysis. When the mechanical properties of Ag/HNTs/PU were tested using a universal strength tester, the results indicated a maximum increase of 109.5% in tensile strength. The researchers then examined the surface roughness and the hydrophobic ability of the Ag/HNTs/PU thin films by using atomic force microscopy and water contact angle. Lastly, antibacterial testing on Escherichia coli revealed that when the additive of Ag/HNTs reached 2.0 wt%, 99.3% of the E. coli were eliminated. These results indicated that the addition of Ag/HNTs into PU could enhance the thermal stability, mechanical properties, and antibacterial properties of PU, implying the potential of Ag/HNTs-02 as biomedicine material.