AbstractInterface engineering is a promising strategy for controlling the Curie temperature (Tc) and perpendicular magnetic anisotropy (PMA) in magnetic 2D van der Waals (2D vdWs)‐based heterostructures. However, establishing high‐quality interface structures in magnetic 2D vdWs/metal stacks, crucial for maximizing interface effects, remains a significant challenge. Here, a Fe5‐xGeTe2/Pt (F5GT/Pt) prototype with a superior interface quality is achieved using a low‐power physical vapor deposition technique. The magnetic properties of the F5GT/Pt heterostructures are strongly influenced by employing the specific physical deposition method. Stable ferromagnetism at 400 K is observed when depositing Pt atoms with relatively high energy, despite the Tc of pristine F5GT being below 300 K. This unexpected high‐temperature ferromagnetism is attributed to the formation of a ferromagnetic alloy at the interface, commonly present in vdWs‐based stacks fabricated through physical deposition but often overlooked. The deposit of Pt atoms with ultralow energy leads to the formation of a unique Fe5‐xGeTe2/Fe3‐xGeTe2 heterojunction at the interface, significantly enhancing the PMA. This work emphasizes the importance of interface structures in vdWs‐based devices, suggesting that controlling the growth process offers an effective approach to construct and engineer vdWs heterostructures, thus improving the performance and introducing new functionalities to spintronic devices.