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A kind of novel two-dimensional magnetic nanocomposites were successfully fabricated via the immobilization of Fe3O4 nanoparticles onto the surface of graphitic carbon nitrogen (g-C3N4) nanosheets by a facile liquid exfoliated method and subsequent solvothermal reaction. The structural, morphological, compositional, thermal and magnetic characteristics of the as-prepared samples were systematically assessed by employing a wide spectrum of characterization techniques. Subsequently, the as-constructed Fe3O4/g-C3N4 composites were exploited to fabricate a stable magnetorheological (MR) suspension, and the rheological performances and sedimentation stability of the designed MR fluid were evaluated through a rotational rheometer and a visual observation method, respectively. The experimental results revealed that the established MR fluid demonstrated an obvious enhancement in sedimentation stability in comparison with that of another a kind of suspension containing carbonyl iron particles. The higher sedimentation stability realized in this MR smart system can be associated primarily with the dispersed Fe3O4/g-C3N4 composite particles with ultrathin sheet-like nanostructure and the reduced density mismatch.