Sol-gel/drop-coated micro-thick TiO2 memristors were investigated and developed for low-power radiation sensing. Devices constructed with coated aluminum (Al) electrodes exhibited unipolar I-V characteristics with dynamic turn-on voltage, and progressive R-OFF/R-ON ratio loss under applied bias. Endurance failure of micro-thick Al/AI stacks is ascribed to gradual passivation of Al surface resulting from an electrically-enhanced oxygen-ion diffusion. By exchanging a single Al contact with higher work function copper (Cu) metal, two distinct superimposed TiO2 phases were formed. The TiO2 coating on Al surface was carbon-contaminated and amorphous, while that on Cu was found to be additionally doped with Cu-(I/II) ions resulting from the corrosion of the surface of the electrode by the amine-based gelation agent. After initial forming, the hybrid stack could achieve a bipolar memristance, with high R-OFF/R-ON (up to 106), and over 10 switching cycles at low-operating voltages (+/- 1 V). The enhanced memristive switching properties of Al/Cu devices are explained via cooperative valence-change/electrochemical-metallization processes, involving migration of oxygen and copper species. The advanced micro-thick TiO2 memristors were exposed to Cs-137 gamma-rays, providing for the first time initial insights into their radiation detection capabilities. The sensing mechanism through these devices could be actuated by synergistic radiation-induced and field-driven photo-electric effects. (C) 2016 Elsevier B.V. All rights reserved.