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The pyroelectric effect and electron spin-state reconfiguration play a critical role in photocatalysis but are seldom investigated. This work is the first to exploit the fluctuating temperature (ΔT) between the cold-hot alternation in photocatalysis to drive the pyroelectric effect and electron spin-sate reconfiguration. FeS2/CuCo2O4(FS/CCO) hollow core-shell heterojunctions were prepared using hydrothermal and heating treatment methods. The FeS2(FS) can generate heat under near-infrared (NIR) light to provide the elevated temperature end required for the pyroelectric effect of CuCo2O4(CCO) under the influence of ΔT. With this thermoelectric and pyroelectric effect, CCO can release surface charges, generating spontaneous polarization, changing the electron (eg) filling number on Co surface sites, reversing the spin electron state, thus controlling the carriers' migration direction and enhancing their separation and migration rate, and finally prolonging their lifetime. As a result, the as-designed FS/CCO-15 composites yielded up to 19.5 mmol g−1h−1extraordinary photocatalytic performance, i.e., 10.2 and 6.45-fold of the pure FS (1.92 mmol g−1h−1) and CCO (3.02 mmol g−1h−1) under simulated sunlight, respectively. It also yielded up to 19.8% average apparent quantum yield. This work thoroughly explored the distinctive impact of the pyroelectric effect, electron spin-state reconfiguration, orbital coupling effect, and hydrogen evolution, guiding us and creating more possibilities for photocatalytic technology and efficiency using NIR light.