A novel hydridobis(silyl)iron(IV) complex Cp*(CO)Fe(H){SiMe2O(2-C5H4N)}(2) (1) (CP*=eta (5)-C5Me5) was synthesized in high yield. Two elimination processes from 1 were effectively controlled by the reaction conditions: HSiMe2O(2-C5H4N) is eliminated on heating or UV-irradiation, whereas HO(2-C5H4N) is eliminated in the presence of Et3Al. The latter reaction was applied to a "silylene introduction" toward a silyl complex producing a silyl(silylene) complex.