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Abstract 2D van der Waals (vdW) magnets with layer‐dependent magnetic states and/or diverse magnetic interactions and anisotropies have attracted extensive research interest. Despite the advances, a notable challenge persists in effectively manipulating the tunneling anisotropic magnetoresistance (TAMR) of 2D vdW magnet‐based magnetic tunnel junctions (MTJs). Here, this study reports the novel and anomalous tunneling magnetoresistance (TMR) oscillations and pioneering demonstration of bias and gate voltage controllable TAMR in 2D vdW MTJs, utilizing few‐layer CrPS₄. This material, inherently an antiferromagnet, transitions to a canted magnetic order upon application of external magnetic fields. Through TMR measurements, this work unveils the novel layer‐dependent oscillations in the tunneling resistance for few‐layer CrPS₄devices under both out‐of‐plane and in‐plane magnetic fields, with a pronounced controllability via gate voltage. Intriguingly, this study demonstrates that both the polarity and magnitude of TAMR in CrPS₄can be effectively tuned through either a bias or gate voltage. The mechanism behind this electrically tunable TAMR is further elucidated through first‐principles calculations. The implications of the findings are far‐reaching, providing new insights into 2D magnetism and opening avenues for the development of innovative spintronic devices based on 2D vdW magnets. 

Abstract Covalent 2D magnets such as Cr₂Te₃, which feature self‐intercalated magnetic cations located between monolayers of transition‐metal dichalcogenide material, offer a unique platform for controlling magnetic order and spin texture, enabling new potential applications for spintronic devices. Here, it is demonstrated that the unconventional anomalous Hall effect (AHE) in Cr₂Te₃, characterized by additional humps and dips near the coercive field in AHE hysteresis, originates from an intrinsic mechanism dictated by the self‐intercalation. This mechanism is distinctly different from previously proposed mechanisms such as topological Hall effect, or two‐channel AHE arising from spatial inhomogeneities. Crucially, multiple Weyl‐like nodes emerge in the electronic band structure due to strong spin‐orbit coupling, whose positions relative to the Fermi level is sensitively modulated by the canting angles of the self‐intercalated Cr cations. These nodes contribute strongly to the Berry curvature and AHE conductivity. This component competes with the contribution from bands that are less affected by the self‐intercalation, resulting in a sign change in AHE with temperature and the emergence of additional humps and dips. The findings provide compelling evidence for the intrinsic origin of the unconventional AHE in Cr₂Te₃ and further establish self‐intercalation as a control knob for engineering AHE in complex magnets.