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Abstract Boron (B) alloying transforms the magnetoelectric antiferromagnet Cr₂O₃into a multifunctional single‐phase material which enables electric field driven π/2 rotation of the Néel vector. Nonvolatile, voltage‐controlled Néel vector rotation is a much‐desired material property in the context of antiferromagnetic spintronics enabling ultralow power, ultrafast, nonvolatile memory, and logic device applications. Néel vector rotation is detected with the help of heavy metal (Pt) Hall‐bars in proximity of pulsed laser deposited B:Cr₂O₃films. To facilitate operation of B:Cr₂O₃‐based devices in CMOS (complementary metal‐oxide semiconductor) environments, the Néel temperature,T_N, of the functional film must be tunable to values significantly above room temperature. Cold neutron depth profiling and X‐ray photoemission spectroscopy depth profiling reveal thermally activated B‐accumulation at the B:Cr₂O₃/ vacuum interface in thin films deposited on Al₂O₃substrates. The B‐enrichment is attributed to surface segregation. Magnetotransport data confirm B‐accumulation at the interface within a layer of ≈50 nm thick where the device properties reside. HereT_Nenhances from 334 K prior to annealing, to 477 K after annealing for several hours. Scaling analysis determinesT_Nas a function of the annealing temperature. Stability of post‐annealing device properties is evident from reproducible Néel vector rotation at 370 K performed over the course of weeks.