Owing to their tunable bandgap with the concentration of the Mg dopant, magnesium−zinc oxide (Mg x Zn (1−x) O) ternary nanometer-thick thin films have been widely studied for applications in the fields of microelectronics and optoelectronics. There are a few reports about the promise of using atomic layer deposition (ALD) to synthesize Mg x Zn (1−x) O for applications in photovoltaics. The synthesis−structure−property relationship of Mg x Zn (1−x) O ALD thin films is not yet clear. In this work, we present a systematic study about the growth behavior of Mg x Zn (1−x) O nanometer thin films by ALD by using in-situ quartz crystal microbalance analysis and a set of ex-situ analyses. We employed diethylzinc (DEZ), biscyclopentadienyl-magnesium (MgCp 2 ), and H 2 O as the precursors for ZnO and MgO ALD chemistries in our study. We find that the nucleation of ZnO on the MgO-doped ZnO surface can be accelerated at 200 °C but be delayed at 120 °C in the growth of Mg x Zn (1−x) O. The crystal structure and optical properties of Mg x Zn (1−x) O ALD films are also different at growth temperatures of 200 and 120 °C. Such understanding can help rationally choose the deposition conditions for ALD Mg x Zn (1−x) O nanoscale thin films in various applications.