The electrochemical intercalation is one of most powerful tools for tuning the intrinsic properties of quasi-two-dimensional (2D) materials. In this work, ionic organic cations, \([\hbox {C}_2\hbox {MIm}]^+\) and \(\hbox {[DEMB]}^+\) , are successfully intercalated into \(\hbox {NiPS}_3\) interlayer via electrochemical intercalation. The both \([\hbox {C}_2\hbox {MIm}]^+\) and \(\hbox {[DEMB]}^+\) intercalated \(\hbox {NiPS}_3\) samples show ferrimagnetic transition with the transition temperature of 65 K and 85 K, respectively. Raman spectroscopy, X-ray photoelectron spectroscopy and Hall measurements reveal that the electron doping and sulfur vacancies created by the cation intercalation play important role in the ferrimagnetic transition. Our work provides a new pathway to manipulation of magnetism in layered 2D materials.
