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Nanostructured (Sm,Pr)(Co,Zr) magnets with the TbCu7-type structure have been synthesized by mechanically milling (Sm1-xPrx)12.5Co85.5Zr2 alloys (0≤x≤0.8) followed by appropriate annealing. Magnetic properties, structure, and microstructure have been investigated. It is found that single-phase (Sm,Pr)(Co,Zr) 7 magnets with the TbCu7 structure and with nanoscale grain size (14–19 nm) form in the whole composition range. Intrinsic coercivity Hci decreases from 20.7 to 5.6 kOe with increasing Pr content from 0 to 0.8, while energy products (BH)max shows an optimum value of 12.6 MGOe (Hciof 17.9 kOe) at x = 0.2 due to increase in remanent magnetization. Remanence ratio is observed in the range of 0.64–0.69, with an optimum value of ~0.69 at x = 0.3. The high coercivity is ascribed to the formation of nanocrystalline (Sm,Pr)(Co,Zr) 7 phase of the TbCu7-type structure with large anisotropy, and the remanence enhancement may result from the exchange-coupling interactions between nanosized (Sm,Pr)(Co,Zr)7 grains. The magnetic properties can be understood in term of the anisotropy of the magnetically hard phase and the interactions between the nanosized grains.