To achieve the color calibration in the multi-spectral image print output, a new calibration method for the multi-ink printer is proposed. By sampling in the multi-ink print color space, measuring the spectral reflectance of the samples and then transforming the reflectance data to a low-dimensional spectral space, a forward look-up table is established firstly. Then by sampling in the low-dimensional spectral space and using the nonlinear optimization to determine the mapping points of the samples in the printer color space, a backward look-up table is created. Meanwhile, optimization parameters are determined according to the samples, which improves the optimization accuracy and shortens the computing time. Finally a multi-linear interpolation method is carried out on the forward and backward look-up table to achieve the spectral color calibration of the multi-ink printer. Experiments show that compared with the spectral color calibration model methods, the new method increases the colorimetric and spectral precision by 40% and 44%, respectively, in forward calibration, and 51% and 41% in backward calibration. The time efficiency is improved by 96% in backward calibration.