Electrical control of magnetism of two-dimensional (2D) antiferromagnetic (AFM) materials combines the advantages of controlling magnetism by purely electrical means, compatibility with semiconductor process, low energy consumption, heterogeneous integration of 2D materials with van der Waals (vdW) interface, and AFM materials with no stray field, resistance to external magnetic field interference, and high intrinsic frequency, and thus becomes a research focus in the field. The carrier concentration control is the main mechanism of electrical control of magnetism, and has been proved to be an effective way to control the magnetic properties of materials. The intralayer-antiferromagnetic materials have net-zero magnetic moments, and it is a challenging task to measure their regulated magnetic properties. Therefore, there is limited research on the electrical control of magnetism of intralayer-antiferromagnetic materials, and their potential mechanisms are not yet clear. Based on the diversity of organic cations, the present work systematically modulates the carrier concentrations of 2D intralayer-antiferromagnetic materials MPX₃ (M = Mn, Fe, Ni; X = S, Se) by utilizing organic cations intercalation, and investigates the influence of electron doping on their magnetic properties. Phase transitions between AFM-ferrimagnetic (FIM)/ferromagnetic (FM) depending on carrier concentration changes are observed in MPX₃ materials, and the corresponding regulation mechanism is revealed through theoretical calculations. This research provides new insights into the carrier-controlled magnetic phase transition of 2D magnetic materials, and opens up a pathway for studying the correlation between the electronic structure and magnetic properties of 2D magnets, and designing novel spintronic devices as well.