The NMR chemical shifts of vanadium (V-51) in (imido)vanadium-(V) dichloride complexes with imidazolin-2-iminato and imidazolidin-2-iminato ligands were calculated by the density functional theory (DFT) method with GIAO. The calculated V-51 NMR chemical shifts were analyzed by the multiple linear regression (MLR) analysis (MLRA) method with a series of calculated molecular properties. Some of calculated NMR chemical shifts were incorrect using the optimized molecular geometries of the X-ray structures. After the global minimum geometries of all of the molecules were determined, the trend of the observed chemical shifts was well reproduced by the present DFT method. The MLRA method was performed to investigate the correlation between the V-51 NMR chemical shift and the natural charge, band energy gap, and Wiberg bond index of the V=N bond. The V-51 NMR chemical shifts obtained with the present MLR model were well reproduced with a correlation coefficient of 0.97.