In quantum materials, nonlinear optical responses are highly sensitive to electronic structure and many-body interactions. Probing and manipulating such nonlinear processes is a complex and subtle endeavor, yet it offers deep insights into emerging physics and functionalities. Here, we report an anomalous ultrafast enhancement of second harmonic generation (SHG) in a strongly correlated cobaltite YbBaCo4O7. Above-bandgap femtosecond pumping increases SHG intensity by up to 60 % within 200 fs, with the enhancement persisting for tens of picoseconds. The enhancement is strongly anisotropic, with substantial amplification of in-plane susceptibility tensors, whereas the out-of-plane counterpart shows negligible change. We attribute these anomalies to ultrafast photodoping-induced modulation of the on-site Coulomb repulsion, which dynamically renormalizes the band structure and selectively amplifies specific ^{(2)} components. These nonlinear dynamics encode rich information about the orbital symmetries and energies of the states involved, opening new avenues for all-optical probing of electronic structure in strongly correlated materials.