CFRP can effectively serve as buckle arrestors for subsea pipelines in virtue of the advantages of lightweight, high strength, and corrosion resistance. In this paper, the interface bonding tests were firstly carried out to assess the bonding performance between the CFRP and pipelines. Three types of tests were designed to evaluate the circumferential, axial, and radial bonding properties, respectively, covering the double-strap joint shear test, axial tensile test, and normal tensile test. The stress-bonding slip responses were measured and various failure modes were identified. The effect of CFRP thickness, type of adhesive, adhesive thickness, and interface roughness on the interface bonding property was explored. Subsequently, SS304 pipe specimens wrapped with CFRP buckle arrestors were tested in a hyperbaric vessel. The pressure-variation in volume curves were obtained, and the flattening and U-shape modes were observed. The influences of adhesive type, adhesive thickness, interface roughness, number of CFRP layers, CFRP thickness, and CFRP length on the crossover pressure were examined. The results demonstrate that the number of CFRP layers and CFRP thickness remarkably affect the arresting performance of CFRP arrestors, and the influence of interface bonding properties on the arresting ability is not as significant as the adhesive strength.