A series of complex HfO 2 /Al 2 O 3 layer by layer resistive random access memory(RRAM) structure grown by atomic layer deposition are investigated. The modulation of forming voltage can be achieved by controlling the number of Al 2 O 3 layers in HfO 2 devices. In addition, the crystallization temperature of HfO 2 based RRAM devices can also be improved by insetting Al 2 O 3 layers in HfO 2 film. Compared with pure HfO 2 device, a significant improvement in resistive switching properties such as forming voltage variation and the distribution of HRS/LRS during resistance switching is demonstrated in the HfO 2 /Al 2 O 3 layer by layer devices. Moreover, good endurance characteristic and highly reliable multibit operation are also achieved in this device structure.Resistive random access memory (RRAM) is a promising candidate to replace the currently flash memory device due to its simple structure, low voltage operation, high scalability, and multibit data storage. 1,2 It is found that transition metal oxides (TMOs) can be utilized in RRAM devices, such as ZrO 2 , 3,4 NiO, 5 and HfO 2 . 6-11 Among those various TMOs, HfO 2 is one of the appealing materials that had considerable attention owing to its high dielectric constant (k), superior resistive switching (RS) performance, and compatible standard complementary metal oxide semiconductor (CMOS) technology process. 6 However, the thermal stability of HfO 2 thin film is a serious issue for memory characteristics due to the low crystallization temperature (<400 • C). 12 The RRAM devices with crystalline phase HfO 2 film suffer the RS behaviors variation due to location dependent conductive filament (CF) formation. For example, if CF grows along the grain boundaries of polycrystalline HfO 2 film, low forming voltage and good RS behaviors are observed, whereas high forming voltage is detected in amorphous phase and crystalline phase HfO 2 RRAM devices. 7 On the other hand, crystalline phase HfO 2 film, which is stoichiometric structure, prevents creating enough oxygen vacancies in RRAM devices for RS behaviors. 8 Moreover, the high forming voltage crystalline phase HfO 2 film may cause RRAM devices hard breakdown during forming process. Besides, for the scaled RRAM devices, the larger non-uniformity grain boundaries for cell by cell with crystalline phase HfO 2 film will cause the variation of device performance. 9 Therefore, the amorphous phase HfO 2 exhibiting uniformity film quality is suitable for RRAM development. According to previous literature, the RS behaviors are dependent on the degree of crystalline of HfO 2 film, which critically influences the device yield. Hence, this phenomenon of low crystallization temperature in HfO 2 is not allowed existence in further RRAM applications.In this letter, we fabricate Hf x Al y O films, which are the architecture with a series of complex HfO 2 /Al 2 O 3 layer by layer structure by using atomic layer deposition system (ALD), for HfO 2 -based RRAM devices. Here, we show the insetting Al 2 O 3 layers would significantly in...