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Rapidly solidified Al87Ni7Cu3Nd3 metallic glasses, prepared by using melt spinning, were treated under both isothermal and non-isothermal regime. The amorphous rib-bon and the annealed samples were closely examined by means of differential scan-ning calorimetric, conventional X-ray diffraction and high resolution transmission electron microscopy with selected-area electron diffraction, with special interest in pri-mary crystallization into α-Al nanocrystalline particles, in order to understand struc-tural characteristics of Al-based amorphous/nanocrystalline alloys, and nucleation and grain growth mechanism on the nanometer scale during primary crystallization. The results show that, the as-prepared ribbons are fully amorphous and homogeneous in the micron scale, but contain high density of quenched-in clusters or crystallite embryos. Primary crystallization mainly leads to formation of two-phase mixture of α-Al crystal and residual amorphous phase. The annealed ribbons exposed isother-mally at 110℃ for 5, 130 minutes and heated continuously up to less than 310℃ at 40℃/min consist of large amount of α-Al fec crystal nanoparticles dispersed uni-formly in an amorphous matrix. However, a very little amount of finer orthorhombic Al3Ni intermetalics particles exist in the annealed ribbons heated up to 310℃. During primary crystallization, the leading kinetic mechanics to impede growth of the α-Al crustal is soft impinaement, instead of geometric impinqement.