Organosilyl ammonium borohydride(2_) was synthesized via route of sol-gel process of organosilyl ammonium chloride(1_), The mole ratio of 1/1/4/2/1.O×10^(-2) of 3-chloropropyltriethoxysilane/dimethyldodecylamine/H₂O/THF/HCl(cat) was proved as an optimal condition on the synthesis of organsilyl quarternary ammonium chloride. In borohydration reaction of organosilyl quarternary ammonium chloride, the prduction of organosilyl quarternary ammonium borohydride was identified by B-H stretching vibrations of 2371, 2320, 2274 cm^(-1) on a vibrational spectroscopy. As a result, the intent of RH_4^- was found to be 2.0 mmol per one gram of organosilyl quarternary ammonium borohydride.