The purpose of this study is to evaluate the optimal earthquake intensity measures (IMs) for probabilistic seismic demand models (PSDMs) of the base-isolated nuclear power plant (NPP) structures. The numerical model of NPP structures is developed using a lumped-mass stick model, in which a bilinear model is employed to simulate the force-displacement relations of base isolators. In this study, 20 different IMs are considered and 90 ground motion records are used to perform time-history analyses. The seismic engineering demand parameters (EDPs) are monitored in terms of maximum floor displacement (MFD), the maximum floor acceleration (MFA) of the structures, and maximum isolator displacement (MID). As a result, a set of PSDMs of the base-isolated structure is developed based on three EDPs (i.e., MFD, MFA, and MID) associated with 20 IMs. Four statistical parameters including the coefficient of determination, efficiency (i.e., standard deviation), practicality, and proficiency are then calculated to evaluate optimal IMs for seismic performances of the isolated NPP structures. The results reveal that the optimal IMs for PSDMs with respect to MFD and MID are velocity spectrum intensity, Housner intensity, peak ground velocity, and spectral velocity at the fundamental period. Meanwhile, peak ground acceleration, acceleration spectrum intensity, A95, effective peak acceleration, and sustained maximum acceleration are efficient IMs for PSDMs with respect to MFA of the base-isolated structures. On the other hand, cumulative absolute velocity is not recommended for determining the exceedance of the operating basis earthquake of base-isolated NPP structures.