The large uniaxial magnetic anisotropy energy ) [1,2] of Fe-Pt alloys makes their nanostructured forms attractive for potential use as nanoscale magnetic bits in ultrahigh-density information storage devices [3][4][5][6][7] or as fillers to create new types of magnetocomposites. The high magnetic anisotropy and coercivity arise from the chemically ordered face-centered-tetragonal (fct) L1 0 phase, which is sensitive to both chemical composition and the size of the nanoparticles. [4,8,9] Control over particle size and dispersity [10][11][12][13] is essential to form ordered arrays of nanoparticles, and preserve these features against agglomeration [14,15] during high-temperature annealing (e.g., 550°C) treatments used to obtain the L1 0 phase. Therefore, it is crucial to develop protocols to produce FePt nanoparticles with control over composition, particle size, and dispersity, and thermal stability for exploiting their assemblies for data-storage media applications. The synthesis technique described here is a promising approach to realize all these features simultaneously.Prior works have demonstrated FePt nanoparticles synthesis with either excellent size control [3][4][5]10,16] or chemical compositional control [17][18][19] but not both. Thermal decomposition of Fe(CO) 5 vapor, and reduction of Pt(acac) 2 , produces monodisperse nanoparticles with tunable sizes in the 2-15 nm range. [3][4][5]20] But, the chemical composition of the nanoparticle is different from the initial molar ratio of the metal precursors due to different precursor decomposition rates.[10] Size control is further complicated by the strong influence of parameters such as Ar gas flow rate, heating rate, and temperature.[ [19] of the initial molar ratio of the metal precursors, but the particle size is constrained to a limited range of approximately 3-5 nm. Neither of these two synthesis routes is easily amenable to coating the nanoparticles with a protective shell of a thermally stable material (e.g., silica or titania) that could prevent particle shape and size changes during postsynthesis annealing for obtaining the L1 0 phase. Although a Fe 3 O 4 shell can be formed [15] by the thermal decomposition method, the shell degrades at temperatures less than 600°C and destroys the nanoparticle structure and shape. Techniques to coat a silica shell on clusters of magnetic nanoparticles that have been presynthesized using a separate processing method have been demonstrated, [21][22][23] but these techniques are not well suited for creating organized assemblies of well-separated nanoparticles for recording media applications. Here, we report the room-temperature synthesis of monodisperse FePt nanoparticles with tunable particle size over an extended range of 4-20 nm and excellent compositional control using microemulsions. We further use the same microemulsion to enhance the nanoparticle thermal stability by forming a 2 nm thick silica shell, which is also used for functionalization with organosilanes. Organized assemblies formed from the molecul...