The anisotropic diamagnetic Kepler problem (ADKP) is realized experimentally by the orbital electrons of a P donor in Si under magnetic fields. The interference of electron wave packets which leads to quasi-Landau resonances (QLR) were observed. Applying the closed-orbit theory to an anisotropic solid state environment, we have identified orbits responsible for the QLR manifesting the quantum chaotic behavior in Rydberg atoms. The excellent consistency between the measured spectra and theoretical calculation provides unambiguous evidence of quantum chaotic dynamics of electrons in the ADKP.