While great progress has been made in the synthesis, property optimization, and applications of chemically synthesized functional nanoparticles (NPs), a signifi cant remaining challenge is to uniformly control the composition and phase of multicomponent NPs. Phase equilibria for NPs may be altered from bulk behavior due to the higher proportion of surface atoms and contributions from surface chemistry, such as ligand monolayers, resulting in altered thermodynamic and metastable phases for NPs. For Co [ 1,2 ] and Ag, [ 3 ] new phases have been observed in NPs and nanowires, respectively. There have also been several reports of non-equilibrium phases in semiconductor NPs. [4][5][6][7] For multicomponent metal NPs, metastable phases [8][9][10][11] are well known. In some instances, metastable phases frustrate efforts to obtain equilibrium phases. FePt NPs are such a system, wherein an undesired metastable alloy phase and multiple intermetallic phases have hindered the preparation of intermetallic, phase-pure, chemically synthesized FePt NPs with a monodisperse size distribution. [ 12 ] New insights about these challenges and how to overcome them will also be applicable to other kinds of multicomponent metal NPs.FePt NPs are of interest for bit-patterned media (BPM), a prospective architectural paradigm shift for the magnetic recording industry that overcomes the storage density limits of current recording media by using discrete magnetic bits rather than continuous media. [ 13 ] While reducing the bit size increases the storage density, it also increases bits' susceptibility toward thermal demagnetization, which would cause data loss. Superparamagnetism occurs when thermal energy ( k B T ) is suffi cient to overcome a NP's magnetocrystalline anisotropy energy ( KV ), where K is the magnetocrystalline anisotropy constant and V is the volume, which induces random reorientation of the magnetization direction. Magnetocrystalline anisotropy is the coupling of the moment to a favored crystal direction. Other magnetic anisotropies are known, such as those arising from the NP surface, anisotropic shapes, or strain, but for unstrained NPs of approximately spherical shape, magnetocrystalline anisotropy is usually the predominant magnetic anisotropy. The L1 0 intermetallic phase of FePt has an extremely large K of ≈ 10 7 erg cm −3 , [ 14 ] which makes is attractive for BPM, as well as for permanent magnet applications. [ 12 ] In addition to thermal stability, another requirement for BPM is for the variance in the fi eld required to change the magnetization direction of the bits (commonly referred to as the switching fi eld distribution) to be small, in order to avoid high rates of read and write errors. [ 15 ] A narrow switching fi eld distribution can be achieved with periodically spaced bits that have similar magnetic properties. [16][17][18] Monodisperse FePt NPs synthesized using wet-chemical approaches are stabilized by ligands that facilitate self-assembly into highly ordered structures. [ 8 ] Such methods produce disord...