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We have reported tetradentate ligands (salophen) coordinated with N and O atoms that led to the Cu (II) complexes. These Cu (II) complexes (C-1 and C-2) were firstly established by using elemental analysis and confirmed by mass spectra. At the same time, the characterization of C-1 and C-2 complexes is performed by using several spectroscopic methods and morphological analysis. The bandgap values of the C-1 and C-2 complexes are evaluated with UV-vis DRS spectra. The PL spectral data and photocurrent curves clearly indicated the small recombination rate of the hole–electron pair. The synthesized C-1 and C-2 complexes’ photocatalytic properties were examined for the degradation of cationic dyes such as methylene blue (MB λ_max.= 654 nm) and methyl violet (MV λ_max.= 590 nm) below visible-light action. The C-2 complex is more active than the C-1 complex because of its high photostability, small band-gap energy, and low recombination rate for hole–electron pair separation, and improved visible-light character, which encourages the generation of hydroxyl radical species throughout the photodegradation process. Scavenger probes were used to identify the dynamic species for the photodegradation of dyes, and a mechanism investigation was established.