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A salicyaldimine ligand, 3-tert-butyl-4-hydroxy-5-(((pyridin-2-ylmethyl)imino)methyl)benzoic acid (H₂L_salpyca) and two Cu(II)−salicylaldimine complexes, [Cu(HL_salpyca)Cl] (<b>1</b>) and [Cu(HL_salpyca)(NO₃)]<i>_n</i> (<b>2</b>), have been synthesized. Complex <b>1</b> has a discrete mononuclear structure, in which the Cu(II) center is in a distorted square-planar geometry made up of one HL_salpyca⁻ monoanion in an NNO tris-chelating mode and one Cl⁻ anion. Complex <b>2</b> adopts a neutral one-dimensional zigzag chain structure propagating along the crystallographic [010] direction, where the Cu(II) center suits a distorted square pyramidal geometry with a <i>τ</i> value of 0.134, consisted of one HL_salpyca⁻ monoanion as an NNO tris-chelator and two NO₃⁻ anions. When the Cu∙∙∙O semi coordination is taken into consideration, the nitrato ligand bridges two Cu(II) centers in an unsymmetrical bridging-tridentate with a <i>μ</i>, <i>κ</i>⁴O,O′:O′,O″ coordination. Clearly, anion herein plays a critical role in dominating the formation of discrete and polymeric structures of copper salicyaldimine complexes. Noteworthy, complex <b>2</b> is insoluble but highly stable in H₂O and various organic solvents (CH₃OH, CH₃CN, acetone, CH₂Cl₂ and THF). Moreover, complex <b>2</b> shows good photocatalytic degradation activity and recyclability to accelerate the decolorization rate and enhance the decolorization performance of acid orange 7 (AO7) dye by hydrogen peroxide (H₂O₂) under daylight.