Since it offers high specific strength and superior corrosion resistance, nanocrystalline Ni deposits have attracted much attention as a brand-new functional coating used in electrocatalysis and high-temperature oxidation resistance devices. Herein two-directional of horizontal (UF1: 70 kHz) and vertical (UF2: 25 kHz) ultrasonic fields was designed for Ni deposits, establishing the correlation between grain size-dependent micro structures and properties of Ni nanocrystals under the varying ultrasound frequency (UF) from 0 to 70 kHz, respectively. Under the action of two-directional ultrasonic micro jets, the electroplating dendrites along the directional of electric-field density line was sufficiently crushed by impulse waves in UF1, followed by ultrasonic-shattering smaller grains that returned into growing sites for layer-by-layer epitaxial growth in vertical (UF2), resulting in effects of "nucleation and increments''. Experimental evidences indicated that the surface toughness of Ni deposits had great improved under a varied UF value of 25 + 70 kHz (in a ratio of 2:5). The largest Young's modulus (Er) and hardness (HG) value of similar to 22.4 and 198.6 GPa were tested for Ni deposits at 25 + 70 kHz, and followed by a single UF value at 25, 75 and 0 kHz, which was ascribed to such structural modifications and refinement effects by ultrasound disruptions. With an increasing UF from 25 into 70 kHz, structural alterations converted from elliptical-like compact structure into unidirectional columnar with terrace-like textures of Ni deposits. As predicted, the diversified orientations like Ni (220) (200) and (311) plane were transformed from the close-packed Ni (111) plane in fcc-Ni deposits. Besides a lowest friction coefficient of similar to 0.25 was recorded for Ni deposits at UF 25 + 75 kHz without lubricants, reducing by 1.5 times relative to that of Ni sample without ultrasound field. The ultrasound-shattering mechanisms involved in the crystallographic textures and ionic polarization of Ni nanocrystals were explored in detail.