Ni1.5Mg1.5Al1-LDH/GO composite was synthesized by the co-precipitation method, and Ni1.5Mg1.5Al1-LDH/GO/g-C3N4 composites (NCG-X, X = 1, 3, 5) with varying mass ratio of GO to Ni1.5Mg1.5Al1-LDH/g-C3N4 were further constructed using electrostatic self-assembly technology. The photocatalytic degradation performance of the NCG-X composites toward ciprofloxacin (CIP) were influenced by the GO dosage, which regulated the microstructure, light-absorbing ability, and photo-electrochemical characteristics of the NCG-X composites. Compared to the pure g-C3N4 nanosheets and Ni1.5Mg1.5Al1-LDH/g-C3N4 composite, all NCG-X composites exhibited better photocatalytic performance. As the GO dosage raising, the photocatalytic performance of NCG-X composites initially improved but subsequently declined, and the NCG-3 composite (with GO dosage of 3 wt%) achieved the optimum photocatalytic performance. After 120 min of irradiation under visible light, 82.96% of CIP molecules (100 mL, 10 mg/L) were degraded by 0.03 g NCG-3 composite, whose reaction rate constant (0.01237 min-1) was 5.11, 2.35 and 1.75 times that of g-C3N4 nanosheets, MgAl-LDH/g-C3N4 composite and Ni1.5Mg1.5Al1-LDH/g-C3N4 composites, respectively. ·O2- and h+ were the predominant active species during the photocatalytic degradation process. Moreover, NCG-3 composite exhibited excellent universality for degrading organic contaminants like methyl orange, crystal violet, tetracycline, and methylene blue. This work provides a novel strategy for synthesizing high performance LDH/g-C3N4 composite photocatalyst via the modification of GO, and demonstrates the good perspective application of Ni1.5Mg1.5Al1-LDH/GO/g-C3N4 composite for the removal of organic pollutants in wastewater.