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Translating the surging interest in neuromorphic electronic components, such as those based on nonlinearities near Mott transitions, into large‐scale commercial deployment faces steep challenges in the current lack of means to identify and design key material parameters. These issues are exemplified by the difficulties in connecting measurable material properties to device behavior via circuit element models. Here, the principle of local activity is used to build a model of VO₂/SiN Mott threshold switches by sequentially accounting for constraints from a minimal set of quasistatic and dynamic electrical and high‐spatial‐resolution thermal data obtained via in situ thermoreflectance mapping. By combining independent data sets for devices with varying dimensions, the model is distilled to measurable material properties, and device scaling laws are established. The model can accurately predict electrical and thermal conductivities and capacitances and locally active dynamics (especially persistent spiking self‐oscillations). The systematic procedure by which this model is developed has been a missing link in predictively connecting neuromorphic device behavior with their underlying material properties, and should enable rapid screening of material candidates before employing expensive manufacturing processes and testing procedures.

Future‐generation neuromorphic computing seeks to overcome the limitations of von Neumann architectures by colocating logic and memory functions, thereby emulating the function of neurons and synapses in the human brain. Despite remarkable demonstrations of high‐fidelity neuronal emulation, the predictive design of neuromorphic circuits starting from knowledge of material transformations remains challenging. VO₂is an attractive candidate since it manifests a near‐room‐temperature, discontinuous, and hysteretic metal–insulator transition. The transition provides a nonlinear dynamical response to input signals, as needed to construct neuronal circuit elements. Strategies for tuning the transformation characteristics of VO₂based on modification of material properties, interfacial structure, and field couplings, are discussed. Dynamical modulation of transformation characteristics through in situ processing is discussed as a means of imbuing synaptic function. Mechanistic understanding of site‐selective modification; external, epitaxial, and chemical strain; defect dynamics; and interfacial field coupling in modifying local atomistic structure, the implications therein for electronic structure, and ultimately, the tuning of transformation characteristics, is emphasized. Opportunities are highlighted for inverse design and for using design principles related to thermodynamics and kinetics of electronic transitions learned from VO₂to inform the design of new Mott materials, as well as to go beyond energy‐efficient computation to manifest intelligence.