We report the anomalous breakdown in the scaling of the microscopic magnetic susceptibilityas measured via the 31 P nuclear magnetic resonance (NMR) shift K-with the bulk magnetic susceptibility χ in the paramagnetic state of Mn2P2S6. This anomaly occurs near Tmax ∼ 117 K the maximum in χ(T ) and is therefore associated with the onset of quasi-two-dimensional (quasi-2D) magnetic correlations. The spin-lattice relaxation rate divided by temperature (T1T ) −1 in Mn2P2S6 exhibits broad peak-like behavior as a function of temperature, qualitatively following χ, but displaying no evidence of critical slowing down above the Néel temperature TN . In the magnetic state of Mn2P2S6, NMR spectra provide good evidence for 60 degree rotation of stackingfault-induced magnetic domains, as well as observation of the spin-flop transition that onsets at 4 T. The temperature-dependent critical behavior of the internal hyperfine field at the P site in Mn2P2S6 is consistent with previous measurements and the two-dimensional anisotropic Heisenberg model. In a sample of Ni2P2S6, we observe only two magnetically split resonances in the magnetic state, demonstrating that the multiple-peaked NMR spectra previously associated with 60 degree rotation of stacking faults is sample dependent. Finally, we report the observation of a spin-flop-induced splitting of the NMR spectra in Ni2P2S6, with an onset spin-flop field of H sf = 14 T.