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For the first time, HfZrO4 dielectrics deposited with metal-organic chemical vapor deposition (MOCVD) as well as atomic layer deposition (ALD) have been investigated as high-k gate dielectric for 32-nm high-performance logic SOI complementary metal-oxide-semiconductor devices in this letter. The composition of the HfZrO4 films has been analyzed in detail by atom probe tomography, Rutherford backscattering spectrometry, and X-ray photoelectron spectroscopy. Optical inline measurements and electrical parameters such as gate leakage current, capacitance equivalent thickness, threshold voltage, and performance as well as reliability data have been taken into account to directly compare both deposition methods. All parameters indicate a comparable behavior for MOCVD and ALD. Therefore, MOCVD has been demonstrated to be a promising alternative to ALD in high-volume manufacturing.