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Chemical Characterisation of Silanised Zirconia Nanoparticles and Their Effects on the Properties of PMMA-Zirconia NanocompositesObjectives: The objective of this study was to investigate the mechanical properties of high-impact (HI) heat-cured acrylic resin (PMMA) reinforced with silane-treated zirconia nanoparticles. Methods: Forty-five PMMA specimens reinforced with zirconia were fabricated and divided into three groups: Pure HI PMMA (control group), PMMA reinforced with 3 wt.% of non-silanised zirconia nanoparticles and PMMA reinforced with 3 wt.% of silanised zirconia nanoparticles. Silanised and non-silanised zirconia nanoparticles were analysed with Fourier Transform Infrared (FTIR) Spectroscopy. For measuring the flexural modulus and strength, a Zwick universal tester was used, and for surface hardness, a Vickers hardness tester were used. Furthermore, raw materials and fractured surfaces were analysed using Scanning Electron Microscopy (SEM). A one-way ANOVA test followed by a post-hoc Bonferroni test was employed to analyse the data. Results: The results showed that the mean values for flexural strength (83.5 ± 6.2 MPa) and surface hardness (20.1 ± 2.3 kg/mm2) of the group containing 3 wt.% treated zirconia increased significantly (p 0.05) in comparison to the specimens in the group containing non-treated zirconia (59.9 ± 7.1 MPa; 15.0 ± 0.2 kg/mm2) and the control group (72.4 ± 8.6 MPa; 17.1 ± 0.9 kg/mm2). However, the group with silanised zirconia showed an increase in flexural modulus (2313 ± 161 MPa) but was not significantly different (p > 0.05) from the non-silanised group (2207 ± 252 MPa) and the control group (1971 ± 235 MPa). Conclusion: Silane-treated zirconia nano-filler improves the surface hardness and flexural strength of HI PMMA-zirconia nanocomposites, giving a potentially longer service life of the denture base.