Summary: Based on silsesquioxanes (SSO) derived from the hydrolytic condensation of [3-(glacildoxy)propyl]trimethoxysilane (GPMS), 20 wt-% tetraethoxysilane (TEOS) and titanium tetrabutoxide (TTB), two-layer SSO films were prepared for nanoindentation and nanoscratch tests. The tests were carried out to study the influence of different amounts of TTB in the two-layer hybrid films on hardness (H), elastic modulus (E) and scratch (S) testing profiles. The H profiles of the modified films showed two kinds of H corresponding to the two-layer structure. In the S testing profiles, all final-scan profiles did not absolutely coincide or overlap with the firstscan profiles. All S profiles revealed a fluctuanting characteristic and all S profiles can be divided into two regions in the horizontal displacement, because of the two-layer structure. The film containing an adequate amount of TTB (20 wt-%) was found to possess the largest H and E, as well as the best S resistance.