This chapter experimentally studies the synthesis of typical high-energy combustion agent of organic borohydride (B10H10[(C2H5)4N]2, BHN), bis(dialkyl-5-aminotetrazolium) dodecaborates, cationic polynitrogen heterocyclium decahydrodecaborates (CPHD), dihydrazine-1,2,4,5-tetrazine decahydrodecaborate, energetic caged-carborane derivatives and characterizes them by means of IR, SEM, DSC, TG–DTG, etc. techniques from the particle size and particle size distribution, thermal decomposition and heat of combustion aspects.