Hydrogen molecules are formed in the crystalline silicon treated with hydrogen atoms at substrate temperatures between 180 and 500°C. The vibrational Raman line (Q1) of hydrogen molecule in the hydrogenated crystalline silicon is observed at around 4160 cm-1. The line shape changes with hydrogenation temperature, and is composed of at least two components. The two components are ascribed to hydrogen molecule in two different interstitial sites in crystalline silicon. Each component is much broader than that of hydrogen molecules in gas phase. The line broadening can not be explained by collisional or motional broadening, but is attributed due to the configurations of hydrogen molecule with different orientations in the crystalline silicon.