The structural transformations and magnetic property changes of the Nd16.2FebalCo9.9Ga0.5B7.5 (SG1, SG2) and Nd15.0FebalGa2.0B7.3 (SG3) nanocomposite alloys obtained by melt spinning in the as-quenched state and after annealing at a temperature range of 560–650 °C for 30 min were studied. The methods used were X-ray diffraction analysis, magnetic property measurements, TEM studies, X-ray fluorescence analysis and Mössbauer spectroscopy. Amorphous phase and crystalline phase Nd2Fe14B (P42/mnm) were observed in the alloy after melt spinning. The content of the amorphous phase ranged from 20% to 50% and depended on the cooling rate. Annealing of the alloys resulted in amorphous phase crystallization into Nd2Fe14B and led to the increased coercivity of the alloys up to 1840 kA/m (23.1 kOe) at 600 °C annealing for 30 min. The alloy with the maximum coercivity had a grain size of the Nd2Fe14B phase ≈50–70 nm with an Nd-rich phase between grains.