Ultrathin Al2O3 atomic layer deposition (ALD) films with low pinhole density were fabricated using a deposit and etchback approach. This strategy was able to avoid the pinholes that originated during nonuniform nucleation of Al2O3 ALD films. In this method, an Al2O3 ALD film was deposited to a thickness greater than the desired thickness to reduce the number of pinholes and form a more continuous Al2O3 ALD film. Subsequently, the Al2O3 ALD film was etched back to a smaller thickness using thermal Al2O3 atomic layer etching (ALE). The number of pinholes in the resulting Al2O3 ALD film was measured by the percentage yield of metal-insulator-metal (MIM) capacitors based on an Ag/Al2O3/Al structure that did not have an electrical short. The device yield was improved using the deposition and etchback approach. For example, using device areas of 0.01 mm2, Al2O3 ALD films that were grown to 5 nm in the MIM capacitor gave a yield of 30%–40%. In contrast, Al2O3 ALD films that were grown to 24 nm and then etched back to 5 nm to form the MIM capacitor provided a yield of 65%–75%. This increase in yield of approximately 100% indicates that the deposit and etchback approach can improve the yield of MIM devices based on ultrathin Al2O3 ALD films. Although this method has been previously suggested to improve the quality of ultrathin films, this report is believed to be the first demonstrated application of using the deposit and etchback approach for device fabrication. Additional experiments revealed that a portion of the yield improvement can be attributed to the fluorination of the Al2O3 ALD films that produced a volume expansion when forming AlF3. This expansion may produce a compressive stress that helps to close the pinholes. The dielectric constant was also measured for Al2O3 ALD films versus Al2O3 film thickness. The dielectric constant was the same for as-deposited Al2O3 ALD films and Al2O3 ALD films that were first grown to 24 nm and then etched back to smaller thicknesses. This agreement indicates that the dielectric constant can be understood in terms of a series capacitor model and that Al2O3 ALE does not affect the electrical properties of the Al2O3 films.