Ferromagnetic nanoparticles are important materials for nanotechnology both in practical applications and in fundamental research. The different purposes for which they are used have posed significant challenges in their preparation. For example, the development of highly sensitive magnetoresistive (MR) sensors makes it possible to detect the binding interactions between DNA or protein molecules, which are attached by magnetic beads.[1] To achieve high selectivity and sufficient signal-to-noise ratio, oxidation-resistive ferromagnetic nanomagnets are more favorable than the superparamagnetic microbeads usually used. Nanocomposite exchangespring magnets were expected to have unusually high energy products (BH) max (magnetic flux density times magnetic field strength), which requires the fabrication of crystallographically coherent hard and soft magnetic phases with a proper exchange coupling. [2,3] This requires nanometer-scale structure and property control of both the hard and soft magnetic components. Future extremely high density magnetic storage media demand high anisotropic magnetic materials, such as L1 0 -phase FePt, to overcome the superparamagnetic limit.[4]Chemical ordering and orientation control are essential prerequisites for the popular wet-chemical approach, [5] and these are difficult to achieve by post-deposition annealing. [6] We have recently reported a vacuum technique based on the gasphase condensation principle to prepare directly ordered FePt nanoparticles. [7] Here we present a general methodology of tuning the crystal structure and magnetic properties of FePt binary alloy nanomagnets.The final crystal structure of nanoparticles is a result of their thermal history, which involves both thermodynamic and kinetic factors. The binary phase diagram of equiatomic FePt alloy shows that it has two solid-state phases: fcc disordered (face-centered cubic or A1 phase) and fct ordered (face-centered tetragonal or L1 0 phase), with fcc as the high-temperature stable phase.[8] Many of the preparation techniques are kinetically controlled, so the fcc disordered phase dominates their final products. To get the fct ordered phase post-deposition annealing is generally used. This annealing process is a first-order phase transformation process, which requires nucleation sites for the ordering to originate. In FePt thin films, grain boundaries and crystal defects can supply such starting points for phase transformation. FePt nanoparticles are more difficult to transform because they do not have conventional grain boundaries and do not have many defects either.[9] Accordingly, any post-annealing approach usually results in particle agglomeration and twin formation, which will limit their applications. An alternative, and also optimal, way to prepare nanoparticles with the desired crystal structure is to control the thermal environment for their nucleation and growth, which is the main focus of this work. There are several different ways to control the thermal environment for particle nucleation and growth by ...