For nanomaterials, such as GO and MOF-525, aggregation is the main reason limiting their adsorption performance. In this research, Alg-Cu@GO@MOF-525 was successfully synthesized by in-situ growth of MOF-525 on Alg-Cu@GO. By dispersing graphene oxide (GO) with copper alginate (Alg-Cu) with three-dimensional structure, MOF-525 was in-situ grown to reduce aggregation. The measured specific surface area of Alg-Cu@GO@MOF-525 was as high as 807.30 m2·g−1, which is very favorable for adsorption. The synthesized material has affinity for a variety of pollutants, and its adsorption performance is significantly enhanced. In particular, tetracycline (TC) was selected as the target pollutant to study the adsorption behavior. The strong acid environment inhibited the adsorption, and the removal percentage reached 96.6% when pH was neutral. Temperature promoted the adsorption process, and 318 K adsorption performance was the best under experimental conditions. Meanwhile, 54.6% of TC could be removed in 38 min, and the maximum adsorption capacity reached 533 mg·g−1, far higher than that of conventional adsorption materials. Kinetics and isotherms analysis show that the adsorption process accords with Sips model and pseudo-second-order model. Thermodynamic study further shows that the chemisorption is spontaneous and exothermic. In addition, pore-filling, complexation, π-π stack, hydrogen bond and chemisorption are considered to be the causes of adsorption.