Reasonable ground motion intensity measures are important basis for predicting and evaluating the seismic response of structures. One long-period high-rise frame core tube structure and a single degree of freedom (SDOF) system with 24 periodic points were selected. Based on the time-history analysis results of 100 ground motion records with different focal mechanisms, the correlations between 16 ground motion intensity measures and the structural seismic response were studied, and improved spectral correlation ground motion intensity measures considering the influence of high modes were proposed. The results showed that:(1) The correlations between different ground motion intensity measures and the structural seismic response are quite different. With the increase in natural period of SDOF system, the correlation between intensity measures and the seismic response tend to decrease. (2) According to the analysis of correlations between each intensity measure and seismic responses of the high-rise long-period structure (maximum vertex displacement, maximum base shear, and maximum story drift), the peak ground velocity is recommended as the best intensity measure for high-rise long-period structures. (3) As high-rise long-period structures are significantly affected by high modes, the response spectrum measure with high modes can be used to improve the correlation.