This study proposes a new arrangement-tuning method to maximize the potential of tuned mass dampers (TMDs) in decreasing the seismic responses of tall buildings. The method relies on a Grammian-based entropy index with the physical meaning of covariance responses to white noise without the involvement of external inputs. A twelve-story RC frame-shear wall building was used as an example to illustrate the method. Indices were computed for the building with TMDs placed on different stories and tuning to different modes and were compared with responses to white noise (colored) time histories. Results showed that greater index reduction cases agree well with greater story-drift reductions cases, despite the differences in the time step of the white noises and structural model types (pure shear vs. shear-bending), and the optimal TMD is not necessarily the traditional “roof—1st mode tuning” case. Comparisons were also made for the shear-bending building under seven earthquake excitations. It is found that, though TMDs are not full-band effective controllers, the index-selected TMDs still perform the best in three out of seven earthquakes. So, the proposed internal-property-based entropy index provides a good controller design for large-scale structures under unpredictable none-stationary excitations.