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The development of new‐type memristors with special performance is of great interest. Herein, an inorganic‐organic hybrid crystalline polyoxometalate (POM) with usual dynamic structures is reported and used as active material for fabricating memristor with unique temperature‐regulated resistive switching behaviors. The hybrid POM not only exhibits tunable thermochromic properties, but also thermal‐induced reversible aggregation and disaggregation reactions, leading to reversible structural transformations in SCSC fashion. Further, the memory device using the hybrid POM as active layer exhibits uncommon performance, which can keep resistive switching silent in the low temperature range of 30–150 °C, but show nonvolatile memory behavior in the high temperature range of 150–270 °C. Particularly, the silent and working states at three special temperatures (30, 150 and 270 °C) can be monitored by chromism. The correlation between structure and resistive switching property of the material has been discussed. The work demonstrates that crystalline inorganic‐organic hybrid POMs are promising materials for making memristors with superior performance. [ABSTRACT FROM AUTHOR]

• Memory devices fabricated with protonated g-C 3 N 4 can exhibit enhanced memory performances, in which acid concentration is crucial. • g-C3N4 treated with 8 M HCl presents the best resistive switching performance, which might be relative to its texture without violent tortuosity. • The protonated g-C 3 N 4 -based memory devices present good environmental robustness, including temperature and ionizing irradiation. • The high tolerant temperature (454 °C) can also be enhanced by doping BN for heat dissipation. Memory devices with simple sandwich structures using the g-C 3 N 4 treated by different concentration acids as active layers have been fabricated, which exhibit enhanced non-volatile bipolar switching performances and good environmental robustness. [Display omitted] The searching for new memory that can work under harsh conditions will be significant for their application in some important fields such as geothermal, oil and aerospace industries. In this work, memory devices with simple sandwich structures using the g-C 3 N 4 treated by different concentration acids as active layers have been fabricated, which exhibit non-volatile behaviors and bipolar switching characteristics. Protonation treatment can enhance the memory performance efficiently compared with un-protonized device. Among them, the device containing g-C 3 N 4 treated with 8 M HCl presents the best resistive switching performance with ON/OFF ratio of 104 and good retention capability, which might be relative to its texture without violent tortuosity. In addition, the protonated g-C 3 N 4 -based memory devices exhibit good environmental robustness, including temperature and ionizing irradiation. Specially, its high tolerant temperature (454 °C) can also be assisted by doping BN for heat dissipation. Their good thermal/irradiating stabilities are assigned to the strong bond energy of C N double bonds localized π-conjugated tri-s-triazine rings. In all, the facial protonation treatment without any functionalization or supporting, the simple sandwich device structure and good environmental robustness endow their promising applications in aerospace and outdoor environment. [ABSTRACT FROM AUTHOR]