Combining ferromagnetic–antiferromagnetic materials in nanoalloys (i.e., nanoparticles, NPs, containing more than one element) can create a diverse landscape of potential electronic structures. As a result, a number of their magnetic properties can be manipulated, such as the exchange bias between NP core and shell, the Curie temperature of nanoparticulated samples, or their magnetocaloric effect. In this work, such a family of materials (namely M–Cr NPs where M is Fe, Co, Ni, or some combination of them) is reviewed with respect to the tunability of their magnetic properties via optimized doping with Cr up to its solubility limit. To this end, gas‐phase synthesis has proven a most effective method, allowing excellent control over the physical structure, composition, and chemical ordering of fabricated NPs by appropriately selecting various deposition parameters. Recent advances in this field (both experimental and computational) are distilled to provide a better understanding of the underlying physical laws and point toward new directions for cutting‐edge technological applications. For each property, a relevant potential application is associated, such as memory cells and recording heads, induced hyperthermia treatment, and magnetic cooling, respectively, aspiring to help connect the output of fundamental and applied research with current real‐world challenges.