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A bulk nanocomposite composed of tightly packed self-forming core/shell nanoparticles of metal/oxide was fabricated. The crystalline grain size of the nanoparticles, the packing ratio, and the composition were controlled in the nanocomposite, and their effects on the magnetic properties were investigated. The crystalline grain size of the nanoparticles, the packing ratio, and the composition strongly influenced the magnetic anisotropy field, magnetic coercivity, relative permeability, and loss factor at GHz bands. High permeability with a low loss factor of less than 1.5% at up to 1 GHz was obtained in the nanocomposite in which the nanoparticles with a crystalline grain size of approximately 15 nm were tightly packed.