It has been shown that the maximal correlation between rsfMRI connectivity and behavioral measures occurs along a positive-negative mode direction characterizing the change of the overall goodness of behavior. Here, we had a thorough examination of rsfMRI/MEG connectivity along this positive-negative mode direction. We found that behavioral changes are associated with significant connectivity modulations that are however distinct at the lower-order sensory/motor areas and higher-order cognitive regions. Moreover, this hierarchy-dependent connectivity modulation is similar for rsfMRI and middle-frequency MEG signals, but reversed for gamma-band MEG signals. The findings may provide novel insight into the neural basis of inter-subject behavioral variability.