The angular velocity of Earth's rotation shows decadal oscillations due to the lunisolar gravitational torque, as well as inter- or intra-annual changes arising from the angular momentum exchange between the atmosphere and the solid Earth. The energies involved in the Length of Day (LOD) variations may affect the crustal deformation rate and seismic energy release on a global scale. We found significant correlation between the occurrences of major volcanic eruptions and the LOD pattern since AD 1750. On a multiyear scale, eruption frequency worldwide increases with LOD changes. Moreover, the injection of sulphur gases into the atmosphere during major eruptions is accompanied by significant inter-annual LOD variations. This provides evidence of complex mutual cause-and-effect interactions: stress changes induced by multiyear variations in Earth's spin may affect climactic volcanic activity; also, the atmosphere's dynamic response to volcanic plumes may result in global changes of wind circulation and climate, with consequent LOD variations.