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Utilization of low‐energy photons for efficient photocatalysis remains a challenging pursuit. Herein, a strategy is reported to boost the photocatalytic performance, by promoting low‐energy photons dual harvest through bimodal surface plasmon resonance (SPR)‐enhanced synergistically upconversion and pyroelectricity. It is achieved by introducing triplet–triplet annihilation upconversion (TTA‐UC) materials...