Two-dimensional (2D) materials have provided a fascinating platform for exploring novel multiferroics and emergent magnetoelectric coupling mechanisms. Here, a novel 2D asymmetric multiferroic based on Janus 2D multiferroic MXene-analogous oxynitrides (InTlNO) is presented by using first-principles calculations. We find three inequivalent phases for InTlNO, including two metallic phases (p1 and p2) and one semiconducting phase (p3) with a band gap of 0.88 eV. All phases are room-temperature multiferroics with different Curie temperatures, leading to tunability by phase transitions. We show that there is a 90° rotation of the magnetic anisotropy easy axis between p1 and p2, where p1 favors the in-plane and p2 the out-of-plane easy axis. Therefore, the magnetic anisotropy can be tuned by reversing the out-of-plane polarization. Our strategy provides a unique way toward strong magnetoelectric coupling and multistate memory.