Multifunctional　memristors　with　a　high　memory　density,　low　power　consumption,　flexibility,　programmability,　and　environmental　robustness　are　essential　for　next-generation　memories.　In　this　work,　a　titanocene-polysulfide　complex　(Cp2TiS5)　with　strong　S···S　interactions　and　hydrogen　bonds　was　synthesized　and　integrated　with　TiO2　to　create　a　novel　Cu/TiO2/Cp2TiS5/Ag　memristor.　This　device　shows　bipolar　nonvolatile　memory　performance　with　a　remarkable　ON/OFF　ratio　(104.8),　low　switching　voltages　(VSET,　−0.16　V;　VRESET,　+0.15　V),　and　low　power　consumption　(2.7　×　10-4　μW).　It　exhibits　multilevel　memory　behavior,　flexibility,　optical　modulation　(VSET　decreases　from　−1.35　to　−0.17　V　with　decreasing　irradiation　wavelength),　and　thermal　tolerance　(up　to　200　°C).　The　electron-rich　Cp2TiS5　layer　protects　the　Ag-CFs,　while　TiO2’s　oxygen　vacancies　and　unsaturated　Ti　atoms　interact　with　sulfur　from　Cp2TiS5,　lowering　the　Schottky　barrier　and　facilitating　charge　transport.　This　work　offers　promising　opportunities　in　flexible　memristive　devices　for　neuromorphic　computing　under　extreme　conditions.　©　2025　American　Chemical　Society.