The problem of industrial wastewater treatment still poses a challenge to mankind. Congo red (CGR), a kind of organic dye contaminant, is widely used in textile, papermaking, and other industries, making it necessary to develop effective techniques to remove CGR from wastewater. Herein, ZIF-67 crystals with excellent performance were grown in situ on the surface and internal pore surface of the low-cost and high-stability diatomite-based porous ceramic (DBPC) by the nonuniform nucleation growth method, and the DBPC@ZIF-67 composite was characterized by XRD, FTIR, SEM, and EDS methods. Adsorption experiments of DBPC@ZIF-67 to CGR were carried out, and the results showed a theoretical maximum adsorption capacity of 1351.35 mg/g for CGR on DBPC@ZIF-67 and a removal efficiency of 95.53% for 10 mg/L CGR solution at 25 °C. The adsorption kinetics, adsorption isotherms, and adsorption thermodynamics of DBPC@ZIF-67 on CGR were studied using the quasi-first-order and quasi-second-order kinetic models and the Langmuir and Freundlich adsorption isothermal models. The effects of adsorbent dosage and pH value on the adsorption capacity were also investigated. Besides, the stability and recoverability of the composite were studied by adsorption−desorption experiments.