Separation and correlation of the shift anisotropy and the first-order quadrupolar interaction of spin I = 1 nuclei under magic-angle spinning (MAS) are achieved by the phase-adjusted spinning sideband (PASS) nuclear magnetic resonance (NMR) experiment. Compared to methods for static samples, this approach has the benefit of higher sensitivity and resolution. Moreover, the PASS experiment has the advantage over previous MAS sequences in the ability to completely separate the shift anisotropy and first-order quadrupolar interactions. However, the main drawback of the pulse sequence is the lower excitation bandwidth. The sequence is comprehensively evaluated using theoretical calculations and numerical simulations and applied experimentally to the 2H NMR of a range of paramagnetic systems: deuterated nickel(II) acetate tetrahydrate, deuterated copper(II) chloride dihydrate, and two forms of deuterated oxyhydride ion conductor BaTiO3-xHy. Our results show that despite the issue with broadband excitation, the extracted shift and quadrupolar interaction tensors and the Euler angles relating the two tensors match well with the NMR parameters obtained with static NMR methods. Therefore, the new application of the PASS experiment is an excellent addition to the arsenal of NMR experiments for 2H and potentially 14N in paramagnetic solids.