We have performed electrochemical treatment of the van der Waals antiferromagnetic materials FePS3 and NiPS3 with the ionic liquid EMIM-BF4, achieving significant molecular intercalation. Mass analysis of the intercalated compounds, EMIMx-FePS3 and EMIMx-NiPS3, indicated respective intercalation levels, x, of approximately 27% and 37%, and x-ray diffraction measurements demonstrated a massive (over 50%) enhancement of the c-axis lattice parameters. To investigate the consequences of these changes for the magnetic properties, we performed magnetic susceptibility and 31P nuclear magnetic resonance (NMR) studies of both systems. For EMIMx-FePS3, intercalation reduces the magnetic ordering temperature from TN = 120 to 78 K, and we find a spin gap in the antiferromagnetic phase that drops from 45 to 30 K. For EMIMx-NiPS3, the ordering temperature is almost unaffected (changing from 148 to 145 K), but a change towards nearly isotropic spin fluctuations suggests an alteration of the magnetic Hamiltonian. Such relatively modest changes, given that the huge extension of the c axes is expected to cause a very strong suppression any interlayer interactions, point to the conclusion that the magnetic properties of both parent compounds are determined almost exclusively by two-dimensional (2D), intralayer physics. The changes in transition temperatures and low-temperature spin dynamics in both compounds therefore indicate that intercalation also results in a significant modulation of the intralayer magnetic interactions, which we propose is due to charge doping and localization on the P sites. Our study offers chemical intercalation with ionic liquids as an effective method to control not only the interlayer but also the intralayer interactions in quasi-2D magnetic materials.