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Metal-oxide-semiconductor (MOS) capacitors with Al₂O₃ as a gate insulator are fabricated on cubic silicon carbide (3C-SiC). Al₂O₃ is deposited both by thermal and plasma-enhanced Atomic Layer Deposition (ALD) on a thermally grown 5 nm SiO₂ interlayer to improve the ALD nucleation and guarantee a better band offset with the SiC. The deposited Al₂O₃/SiO₂ stacks show lower negative shifts of the flat band voltage V_FB (in the range of about −3 V) compared with the conventional single SiO₂ layer (in the range of −9 V). This lower negative shift is due to the combined effect of the Al₂O₃ higher permittivity (ε = 8) and to the reduced amount of carbon defects generated during the short thermal oxidation process for the thin SiO₂. Moreover, the comparison between thermal and plasma-enhanced ALD suggests that this latter approach produces Al₂O₃ layers possessing better insulating behavior in terms of distribution of the leakage current breakdown. In fact, despite both possessing a breakdown voltage of 26 V, the T-ALD Al₂O₃ sample is characterised by a higher current density starting from 15 V. This can be attributable to the slightly inferior quality (in terms of density and defects) of Al₂O₃ obtained by the thermal approach and, which also explains its non-uniform dC/dV distribution arising by SCM maps.