computation-in-memory paradigm with new electronic devices when handling data-intensive tasks. [1,2] One important attempt is the recently well explored memristor, [3][4][5] in which the nonlinear dynamics of the device allows on demand modulation of the conductance for direct logic operation while the capability of memorizing the new conductance state enables data storage at exactly the same physical location. [6,7] Eliminating the frequent data fetching and movement between the separated memory and processing units, memristors with the simplicity of a resistor structure can lead to extremely compact crossbar array for highly efficient hardware systems. [8,9] In particular, the elaborate evolution of the conductive filament via local ion motion and electrochemistry including foreign cations (such as Ag + and Cu 2+ injected from electrochemically active metal electrodes) and native oxygen anions or vacancies (O 2− or V O ) are widely used to construct atomic point contacts (APCs) with quantized conductance features. [10][11][12][13][14] The stepwise development of device conductance in the unit of conductance quantum G 0 = 2e 2 /h = 77.5 µS (where e is the elemental charge of electrons and h is the Planck's constant), [10] associated with the continuous yet precise atomic Quantum-level manipulation of atomic configuration offers a excellent platform for the construction of exotic nanostructures that exhibit unusual solid-state physics and electronic properties. One particular example is the memristor, in which the elaborate evolution of atomic point contact via local ionic processes and consequent stepwise device conductance quantization enable bottom-up design of in-memory computing with greatly increased data storage density and more efficient multi-value logic algorithm. In-depth understanding on the physics of atomic reconfiguration is achieved through comprehensive consideration of the thermodynamics and kinetics of nanoionics in memristors, based on which a general protocol of constructing atomic point contact structure with desired quantized conductance is established. Through energy-driven single-atom level oxygen manipulation in the reset process of a Pt/HfO x /ITO structure, up to 32 consecutive quantized conductance states with an interval of half conductance quantum that can be sustained for over 7000 s and tuned 500 times are demonstrated for the first time, not only allowing the physical implementation of ternary logic-inmemory functions, but also providing a universal methodology for building next-generation quantum electronic devices.