Methods of forming composite particles include forming a source material over a plurality of nucleation cores and forming a catalyst material over the source material. Compositions of matter include a plurality of composite particles, each particle of the plurality comprising a plurality of nucleation cores, a source material disposed over the nucleation cores, and a catalyst material disposed over the source material. Methods of forming earth-boring tools include forming a plurality of composite particles, combining the plurality of composite particles with a plurality of grains of hard material, and catalyzing the formation of inter-granular bonds between the composite particles and the grains of hard material to faun a polycrystalline material. The plurality of in situ nucleated grains of hard material and the plurality of grains of hard material may be interspersed and inter-bonded.