This article prepared a series of MIL-53(Fe) implanted carbon spheres derived from resorcinol-formaldehyde resins for rapid adsorption of Ciprofloxacin (CIP) using a facile hydrothermal coupling calcination methodology. Results indicated that MIL53(Fe)@RF-800, which was calcined at 800 °C, demonstrated the highest CIP removal efficiency of up to 95% within 60 min in batch adsorption tests. Moreover, MIL53(Fe) @RF-800 could remove over 95.8% of CIP at an amount of 0.2 mg/L, while both Cl− and HCO3− had a negligible impact on the CIP adsorption. It is noteworthy that when there was NO3− or SO42− in the solution, the impact of CIP adsorption displayed an inhibitory trend overall. In addition, MIL53(Fe)@RF-800 exhibited a broad pH range adaptability (over 95% CIP removal efficiency at pH = 3.0–10.5), even under highly acidic (pH < 3.0) or alkaline (pH > 10.5) conditions, the adsorption capacity for CIP was greater than 85%. In conclusion, this study provides novel insights into the development of highly porous MIL-53(Fe)-based adsorbent for rapid and pH-unrestricted adsorption of antibiotics and offers the possibility of practical engineering applications.