To solve the problem that classical Mutual Information (MI) image registration may lead to local extremum, a registration method for multispectral magnetic resonance images based on Cross Cumulative Residual Entropy (CCRE) was proposed. Firstly, the gray level of reference and floating images were compressed into 5 and 7 bits. Then the Hanning windowed Sinc interpolation was used to calculate the CCRE of 5-bit grayscale images, and the Brent algorithm was used to search the CCRE to get the initial transformation parameters of pre-registration. Finally, the Partial Volume (PV) interpolation was adopted to calculate the CCRE of 7-bit grayscale images, and the Powell algorithm was applied to optimize the CCRE to get final parameters from the pre-registration parameters. The experimental results show that the robustness of the proposed method is improved compared with the CCRE registration of PV interpolation, while the registration time is saved about 90% and accuracy is improved compared with the CCRE of Hanning windowed Sinc interpolation. The presented method ensures robustness, efficiency and accuracy, so it is suitable for multi-spectral image registration.