A new algorithm for determining optimal accelerometer locations is proposed by using a frequency-domain Hankel matrix which is much simpler to construct than a time-domain Hankel matrix. The algorithm was examined through simulation studies by comparing the outcomes with those from other available methods. To compare and analyze the results from different methods, a dynamic analysis was carried out under seismic excitation and acceleration data were obtained at the selected optimal sensor locations. Vibrational amplitudes at the selected sensor locations were determined and those of all the other degrees of freedom were determined by using a spline function. MAC index of each method was calculated and compared to look at which method could determine more effective locations of accelerometers. The proposed frequency-domain Hankel matrix could determine reasonable selection of accelerometer locations compared with the others.