Improper disposal of antibiotics poses significant risks to the aquatic environment. Development of efficient adsorbents for removal of antibiotics in environment is currently an important approach to address this issue. In this study, a series of zeolitic imidazolate framework (ZIF-67) materials with different morphologies were synthesized by adjusting the solvent composition during the synthesis process to investigate their adsorption properties for chlortetracycline hydrochloride (CTC). The results indicate that as the volume ratio of methanol to water decreases, the synthesized ZIF-67 transforms from a rhombic dodecahedral structure to a stacked hexagonal platelet structure which is more favorable for the adsorption of CTC. Based on a detailed investigation of the effects of temperature, solution pH, concentration, and types of impurity ions on the adsorption performance of CTC by ZIF-67 with a stacked hexagonal platelet structure (denoted as ZIF-67-3), the kinetics of the adsorption process indicate that the adsorption process follows both pseudo-second-order kinetic model and Langmuir model. Moreover, ZIF-67-3 (at a dosage of 100 mg·L^-¹) achieved a removal rate of over 90% for CTC (with an initial concentration of 30 mg·L^-1) within 20 min, and the maximum CTC adsorption capacity of ZIF-67-3 could reach 1206.58 mg·g^-1 under neutral conditions. Since ZIF-67-3 primarily adsorbs CTC through interactions such as π-π/π-cation interaction and hydrogen/coordination bonds, belonging to a monolayer chemical adsorption mechanism, ZIF-67-3 facilitates full exposure of active adsorption sites, thus exhibiting superior CTC adsorption performance. In summary, this study reveals the influence of solvent composition during synthesis on the morphology and structure of ZIF-67, elucidates the adsorption mechanism of ZIF-67-3 adsorbent for CTC, and provides theoretical support for the practical application of ZIF-67 in removal of antibiotic pollution.