In conventional designs, sensory systems are segregated from memory and computing units. The conversion and transmission of data from analog sensing domains to digital storage result in inefficient power utilization and increased latency. Here, a multifunctional memristor capable of detecting gamma radiation while also serving as a data storage device and an artificial synapse is reported. Large‐scale integration of oxide‐based memristors for artificial neural networks faces major challenges due to the sneak‐path current issue in crossbar arrays. Consequently, material combinations and fabrication variables significantly shape nanoscale processes, which are essential in determining resistive switching properties and functionalities. Resistive switching in AlFeO3 is studied using different electrode materials (silver (Ag), gold (Au), chromium (Cr), fluorine‐doped tin oxide, and silicon), embedding metal (Ag, Au) nanocrystals to engineer a class of tunable memories capable of functioning as selector, memory, artificial synapse, and dosimeter. Techniques like electrode engineering, nanocrystal seeding, and temperature‐dependent thin film deposition are employed to tune resistive and threshold switching functionalities. Accessing different functionalities requires changing the electrode materials or changing the synthesis conditions of the AlFeO3 resistive switching layer and are not interconvertible in the same device simultaneously. The devices emulate critical neural functions and demonstrate interconversion dynamics between short‐term and long‐term plasticity.