The invention discloses a free-space optical micro-cavity Raman laser sensing device and a sensing method thereof. The sensing device comprises a laser light source, a first focusing object lens, an optical micro-cavity, a second focusing object lens, a first collimating lens, a second collimating lens, a first photoelectric detector, an oscilloscope, a filter sheet, a third focusing object lens, a second photoelectric detector and a base spectrum analyzer. Raman laser of an optical micro-cavity is triggered through free-space frequency-tunable laser, and by observing frequency of beat frequency of the Raman laser, information of nanoscale-dimension particles attached to the surface of the optical micro-cavity is obtained; in the free-space Raman laser sensing technology, a whispering gallery mode and the Raman laser can be directly triggered in the free space through the frequency-tunable laser; and through avoiding the technical problems due to the introduction of an optical fiber taper, the flexibility of the device is improved, and signal to noise ratio is reduced, so that sensitivity of the sensing device is improved, and detection limit is reduced.