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This work reports on the correlation between structure, surface/interface morphology and mechanical properties of pulsed laser deposited (PLD)β-Ga₂O₃films on transparent quartz substrates. By varying the deposition temperature in the range of 25 °C–700 °C, ∼200 nm thick Ga₂O₃films with variable microstructure and amorphous-to-nanocrystalline nature were produced onto quartz substrates by PLD. The Ga₂O₃films deposited at room temperature were amorphous; nanocrystalline Ga₂O₃films were realized at 700 °C. The interface microstructure is characterized with a typical nano-columnar morphology while the surface exhibits the uniform granular morphology. Corroborating with structure and surface/interface morphology, and with increasing deposition temperature, tunable mechanical properties were seen in PLD Ga₂O₃films. At 700 °C, for nanocrystalline Ga₂O₃films, the dense grain packing reduces the elastic modulus E_rwhile improving the hardness. The improved crystallinity at elevated temperatures coupled with nanocrystallinity, theβ-phase stabilization is accounted for the observed enhancement in the mechanical properties of PLD Ga₂O₃films. The structure-morphology-mechanical property correlation in nanocrystalline PLDβ-Ga₂O₃films deposited on quartz substrates is discussed in detail.