The present invention discloses a portable multi-azimuth ultrasonic-assisted vibration rolling device and an application method thereof. The vibration rolling device includes an ultrasonic rolling unit, a hydraulic power unit, a pneumatic cooling unit, a main body frame and an indexing device; an amplitude transformer assembly at the ultrasonic rolling unit comes into rolling contact with the surface of a tooth space of a gear workpiece, the hydraulic power unit is articulated with the main body frame, and the hydraulic power unit is articulated with the horn assembly, the indexing device is provided at the main body frame, and the gear workpiece is mounted at the indexing device. The present invention has the advantages that the device is flexible and portable, enables a transducer to be cooled continuously, and facilitates fixation of a rolling steel ball and adjustment of a station of the gear workpiece.