Due to limitations on the availability of rare earth elements it is imperative that new high energy product rare earth free permanent magnet materials are developed for the next generation of energy systems. One promising low cost permanent magnet candidate for a high energy magnet is α″-Fe16N2, whose giant magnetic moment has been predicted to be well above any other from conventional first principles calculations. Despite its great promise, the α″ phase is metastable; making synthesis of the pure phase difficult, resulting in less than ideal magnetic characteristics. This instability gives way to a slew of possible secondary phases (i.e. α-Fe, Fe2O3, Fe8N, Fe4N, etc.) whose concentrations are difficult to detect by conventional x-ray diffraction. Here we show how high resolution neutron diffraction and polarized neutron reflectometry can be used to extract the phase concentration ratio of the giant magnetic phase from ultra-small powder sample sizes (~0.1 g) and thin films. These studies have led to the discovery of promising fabrication methods for both homogeneous thin films, and nanopowders containing the highest reported to date (>95%) phase concentrations of room temperature stable α″-Fe16N2.