In order to combine the merits of both HfO2 and Al2O3 as high-κ gate dielectrics for CMOS technology, high-κ nanolaminate structures in the form of either Al2O3/HfO2/Al2O3 or Al2O3/HfAlOx/Al2O3 were implemented in pMOSFETs and electrically and microstructurally charachterized. ALD TiN film was used as the metal gate electrodes for the pMOSFETs. After full transistor-processing including a rapid thermal processing step at 930 °C, the HfO2 film in the former nanolaminate was found to be crystallized. In contrast, the HfAlOx layer in the latter nanolaminate remained in the amorphous state. Both types of pMOSFETs exhibited a hysteresis as small as ∼20 mV in C-V characteristics in the bias range of +/− 2 V. They also showed a reduced gate leakage current. The pMOSFET with the Al2O3/HfAlOx/Al2O3 nanolaminate was characterized with a subthreshold slope of 77 mV/decade and a channel hole mobility close to the universal hole mobility curve. The pMOSFET with the Al2O3/HfO2/Al2O3, however, exhibited a subthreshold slope of 100 mV/decade and a ∼30% lower hole mobility than the universal curve.