Abstract Hafnium oxide (HfO 2 )‐based devices have been extensively evaluated for high‐speed and low‐power memory applications. Here, the influence of aluminum (Al) and lanthanum (La) co‐doping HfO 2 thin films on the ferroelectric characteristics of hafnium‐based devices is investigated. Among devices with different La/Al ratios, the Al and La co‐doped hafnium oxide (HfAlAO) device with 4.2% Al and 2.17% La exhibited the excellent remanent polarization and thermostability. Meanwhile, first principal analyses verified that hafnium‐based thin films with 4.2% Al and 2.17% La promoted the formation of the o‐phase against the paraelectric phase, providing theoretical support for supporting experimental results. Furthermore, a vertical ferroelectric HfO 2 memory based on 3D macaroni architecture is reported. The devices show excellent ferroelectric characteristics of 22 µC cm −2 under 4.5 MV cm −1 and minimal coercive field of ≈1.6 V. In addition, the devices exhibit great memory performance, including the response speed of device can achieve 20 ns and endurance characteristic can achieve 10 10 cycles.