Treatment of the bulky metallocene hydride Cp*Zr-2(H)OMes (Cp* = pentamethylcyclopentadienyl, Mes = mesityl) with Piers' borane [HB(C6F5)(2)] and carbon monoxide (CO) gave the formylhydridoborate complex [Zr]-O=CH-BH(C6F5)(2) ([Zr] = Cp*2Zr OMes). From the dynamic NMR behavior, its endergonic equilibration with the [Zr]-O-CH2-B(C6F5)(2) isomer was deduced, which showed typical reactions of an oxygen/boron frustrated Lewis pair. It was trapped with CO to give an O [Zr] bonded borata-beta-lactone. Trapping with carbon dioxide (CO2) gave the respective O [Zr] bonded cyclic boratacarbonate product. These reaction pathways were analyzed by density functional theory calculation. The formylhydridoborate complex was further reduced by dihydrogen via two steps; it reacted rapidly with H-2 to give Cp*Zr-2(OH)OMes and H3C B(C6F5)(2), which then slowly reacted further with H-2 to eventually give [Zr]-O(H) B(H)(C6F5)(2) and methane (CH4). Most complexes were characterized by X-ray diffraction.