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(1) Background Iron tetrasulfophthalocyanine with a large nonlinear optical coefficient, good stability, and high catalytic activity has aroused the attention of researchers in the field of photo-Fenton reaction. Further improvement of the visible light photo-Fenton catalytic activity under circumneutral pH conditions for their practical application is still of great importance. (2) Methods In this paper, iron tetrasulfophthalocyanine (FePcS) and phosphomolybdic acid (PMA) cointercalated layered double hydroxides (LDH) were synthesize