Carbon fiber reinforced polymer (CFRP) blades are often exposed to wild and even harsh environments. The durability of the blade can be greatly improved by adhesively bonding a Ni erosion shield to the leading edge. In a traditional bonding process, the permeation of adhesive is poor at the interface, which gives an insufficient micromechanical interlocking. In this study, ultrasonic vibration was applied during the bonding process of sandblasted Ni plates and CFRP laminates. The values of shear strength were measured by tensile tests to verify the strengthening effect of applying ultrasonication. The cross-section of the bonded interface was characterized by scanning electron microscopy (SEM) and energy-dispersive spectroscopy (EDS), and the surfaces with different treatments were explored by atomic force microscopy (AFM). The cross-sectional morphology and failure model of the samples were investigated. The strengthening mechanism was then studied by a molecular dynamics method. For the simulation of molecular dynamics, the CFRP/Ni bonding interface model was designed using the Materials Studio software package. The Perl scripts were used to simulate the ultrasonic vibration with different frequencies and amplitudes. The results showed that the ultrasonic process could improve the permeability and uniformity of the adhesive, enhancing the micromechanical interlocking effect.