The work aims to improve the surface properties of aluminum alloy and extent the application of amorphous coating. A Zr55Al10Ni5Cu30 amorphous rod in the diameter of 2 mm was used as electrode to prepare amorphous alloy coatings on ZL101 alloy surface by electro-spark deposition technique, argon protection and double-deposition technology. The phase compositions, microstructures, surface morphology and interface characteristics of the deposited coatings were analyzed by X-ray diffraction (XRD), optical microscope (OM), scanning electron microscopy (SEM), energy dispersive spectrometer (EDS) and confocal microscope. From the results, the deposited coatings were dense and uniform with silver gray orange peel and the surface morphologies were typical “splash and sputter” and “crater” features. The root-mean-square deviation of unevenness and roughness on the coating was about 3 μm and thickness was approximately 40 μm. The Zr-based deposition coating was mainly composed of amorphous, ZrO2, Cu8Zr3 and ZL101 substrate phase Al(Si). The amorphous was distributed among crystal phases in form of block or strip. Electro-spark deposition technique is an amorphous coating preparation technology with extremely splendid potential due to high discharging frequency, small discharging area, concentrated energy and fast heating and cooling speed. A 3~4 μm thick transition layer is formed owing to the diffusion of element at the interface of prepared amorphous coating and substrate to guarantee the metallurgical bonding.