Nanocrystalline and amorphous Ga2O3 films (%200 nm) with variable structural quality are produced by sputter-deposition by varying the substrate temperature (T s ¼ 25-700 C). The effect of T s is significant on the microstructure and mechanical behavior of Ga 2 O 3 films. The variation in mechanical behavior studied by nano-indentation and nano-scratch testing reveal distinct trends, which are directly related to the structure and morphology of Ga 2 O 3 films. All the Ga 2 O 3 films deposited at T s < 500 C are amorphous; the amorphous-to-crystalline transformation occurs at T s ¼ 500 C. Ga 2 O 3 films deposited at T s ! 500 C are nanocrystalline, β-phase. The corresponding mechanical characteristics, namely the hardness (H) and elastic modulus (E r ), show a strong correlation with structural characteristics. The H and E r increases from 17 to 27 GPa and 250 to 290 GPa, respectively, with increasing T s from 25 to 700 C. The plasticity index, which is the ratio of H/E r , is almost constant for the Ga 2 O 3 films. The strain-rate sensitivity measurements performed to determine the applicability in practical applications indicate the best performance of size controlled, nanocrystalline Ga 2 O 3 films, which can be mechanically regarded as nano-composite structures. The mechanical characteristics, scratch behavior, and strain rate sensitivity indicate the role of microstructure on the mechanical performance of Ga 2 O 3 films.Gallium oxide exhibits polymorphism. The α, β, γ, δ, and e phases of Ga 2 O 3 are widely known. [16,18,[25][26][27] Among these polymorphs, monoclinic β-Ga 2 O 3 is thermally stable with a band gap of %5 eV and high breakdown field 8 MV cm À1 . [28] β-Ga 2 O 3 exhibits n-type conductivity, which is related to donor centers involving oxygen vacancies and/or impurities. The high thermal stability of β-Ga 2 O 3 (melting point %1900 C) is quite useful in the design and development of high-temperature chemical sensors, which can be readily used in automotive industry and power plants. [2] Furthermore, the high-temperature stability coupled with deep ultraviolet transparency makes Ga 2 O 3 based materials as the potential candidates for chemical sensors in extreme environments and transparent electrodes in UV optoelectronics, photonics, and thin-film transistors. [29][30][31] However, in all these applications, fundamental understanding of the structure, thermodynamic conditions, and mechanical characteristics is the key to achieving enhanced device performance.