Antibiotic-resistant genes (ARGs) and antibiotics were detected in various environmental media. Metal-organic framework materials (MOFs) have great advantages in removing many pollutants in water. However, their microporous structure and poor hydrothermally stability make them difficult to realize efficient adsorption performance of macromolecular pollutants. Therefore, this study is devoted to preparing MOF-derived mesoporous carbon materials with excellent pore structure and stability so as to improve the adsorption performance of macromolecular antibiotics in water. In this study, the surface morphological structure of the MOF material was regulated from the preparation process. Firstly, the template agent formed micelles in the MOF framework, so that self-assembly and crystal growth were carried out under the guidance of cooperative templates. Secondly, the morphological structure of the material surface was modified by high-temperature calcination and surface etching. A series of graphitic carbon material MC-X with tunable mesoporous structure were prepared using Zn-MOF materials as precursors and N-Cetyldimethylamine as template. The pore size and mesoporous ratio of the MC-0.3 material had undergone large changes, the pore size varied from 1.73 nm to 3.94 nm, and the mesoporous ratio transformed from 12.6% to 97.71%. Unexpectedly, the material converted from hydrophilic to hydrophobic, and possessed an ultra-high ceftazidime (CAZ) adsorption capacity of 371.18 mg·g−1. The adsorption mechanisms of CAZ on MC-0.3 were mainly molecular size matching selection, hydrophobic effect and hydrogen bonding. After 5 adsorption-desorption cycles, MC-0.3 could maintain about 90% of the initial adsorption capacity.