In the nanoregime, chemical species can reorganize in ways not predicted by their equilibrium bulk behavior. Here, we engineer Ni-Cr nanoalloys at the magnetic end of their compositional range (i.e., 0-15 at. % Cr), and we investigate the effect of Cr incorporation on their structural stability and resultant magnetic ordering. To ensure their stoichiometric compositions, the nanoalloys are grown by cluster beam deposition, a method that allows one-step, chemical-free fabrication of bimetallic nanoparticles. While full Cr segregation toward nanoparticle surfaces is thermodynamically expected for low Cr concentrations, metastability occurs as the Cr dopant level increases in the form of residual Cr in the core region, yielding desirable magnetic properties in a compensatory manner. Using nudged elastic band calculations, residual Cr in the core is explained based on modifications in the local environment of individual Cr atoms. The resultant competition between ferromagnetic and antiferromagnetic ordering gives rise to a wide assortment of interesting phenomena, such as a cluster-glass ground state at very low temperatures and an increase in Curie temperature values. We emphasize the importance of obtaining the commonly elusive magnetic nanophase diagram for M-Cr (M=Fe, Co, and Ni) nanoalloys, and we propose an efficient single-parameter method of tuning the Curie temperature for various technological applications.