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In this paper, we report on the magnetic properties of isolated nanoparticles and interacting nanochains formed by the self-assembly of Ni nanoparticles. The magnetic properties were studied using superconducting quantum interference device (SQUID) magnetometry and magnetic force microscopy (MFM). We demonstrate that single-domain Ni nanoparticles spontaneously form one-dimensional (1D) chains under the influence of an external magnetic field. Furthermore, such magnetic field-driven self-assembly in conjunction with surface templating produces regular arrays of 1D nanochains with antiferromagnetic intra-chain order. The antiferromagnetic order, which is in striking contrast to what is found for non-interacting nanoparticle assemblies within the chains, can be evidenced from MFM and SQUID measurements.