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The magnetic and mechanical properties of Co-P films with amorphous and nanocrystalline structures synthesized through a new route of combining ultrasonic vibration with multipulse electroplating were studied. The deposited amorphous Co-P film shows excellent soft magnetic properties, whereas the nanocrystalline Co-P film shows weak hard magnetic properties. The interfacial adhesion between the deposited Co-P films and the substrate was investigated by the nanoscratch method. The interfacial binding force of the nanocrystalline Co-P film is much larger than that of the amorphous Co-P film. In addition, the nanoindentation experiments show that the electroplated Co-P films have good mechanical properties.