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Herein, we have taken the Ni-supported ferromagnetic (FM) CrBr3 support (Nix\/CrBr3) to thoroughly investigate the effect of spin-order on electrocatalytic oxygen reduction reaction (ORR) via spin-polarized density functional theory calculations. Specifically, Ni loading induces anti-FM coupling in Ni\u2013Cr, leading to a transition from FM-to-ferrimagnetic (FIM) properties, while Ni\u2013Ni metallic bonds create a robust FM direct exchange, benefiting the improvement of the phase transition temperature. Interestingly, with the increase in Ni loading, the easy magnetic axis changes from out-of-plane (2D-Heisenberg) to in-plane (2D-XY). The adsorption properties of Nix\/CrBr3, involving O2 adsorption energy and configuration, are not governed by the d-band center but strongly correlate with magnetic anisotropy. It is noteworthy that the applied potential and electrolyte acidity triggers spin-order transition phenomena during the ORR and induces the catalytic pathway change from 4e\u2212 ORR to 2e\u2212 ORR with the excellent onset potential of 0.93 V\/reversible hydrogen electrode, comparable to the existing most excellent noble-metal catalysts. 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