Performing ab initio calculations, we reveal that the magnetic anisotropy (MA) and the spin direction of a single adatom can be manipulated with a combination of electric fields and adsorption of molecules. Choosing the Fe adatom on the Cu2N/Cu(001) surface as a typical model system, we show that the MA of the pristine Fe adatom and the Fe adatom with an additional H or F atom adsorption remarkably changes by applying an external electric field. Moreover, we show that the F adsorption leads to the spin-reorientation transition of the Fe adatom from in plane to out of plane. Controlling the magnetization dynamics of a single magnetic adatom by molecule adsorption is demonstrated.