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We report a two-step film-growth process using suboxide molecular-beam epitaxy (S-MBE) that produces Si-doped α-Ga2O3 with record transport properties. The method involves growing a relaxed α-(AlxGa1−x)2O3 buffer layer on m-plane sapphire at a relatively high substrate temperature (Tsub), ∼750 °C, followed by an Si-doped α-Ga2O3 overlayer grown at lower Tsub, ∼500 °C. The high Tsub allows the ∼3.6% lattice-mismatched α-(AlxGa1−x)2O3 buffer with x = 0.08 ± 0.02 to remain epitaxial and phase pure during relaxation to form a pseudosubstrate for the overgrowth of α-Ga2O3. The optimal conditions for the subsequent growth of Si-doped α-Ga2O3 by S-MBE are 425 °C ≤ Tsub ≤ 500 °C and P80% O3 = 5 × 10−6 Torr. Si-doped α-Ga2O3 films grown with this method at Tsub > 550 °C are always insulating. Secondary-ion mass spectrometry confirms that both the insulating and conductive films have uniform silicon incorporation. In conductive films with 1019 ≤ NSi ≤ 1020 cm−3, the incorporated silicon is ∼100% electrically active. At NSi ≤ 1019 cm−3, the carrier concentration (n) plummets. A maximum Hall mobility (μ) = 90 cm2V·s at room-temperature is measured in a film with n = 2.9 × 1019 cm−3 and a maximum conductivity (σ) = 650 S/cm at room-temperature in a film with n = 4.8 × 1019 cm−3. A threading dislocation density of (5.6 ± 0.6) × 1010 cm−2 is revealed by scanning transmission electron microscopy, showing that there is still enormous room to improve the electrical properties of doped α-Ga2O3 thin films.