Comprehensive SummaryRationally developing efficient and durable bifunctional catalysts toward oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is critical for rechargeable zinc‐air batteries (ZABs). Herein, a bead‐like CoSe2@NC@NCNFs bifunctional catalyst was designed and fabricated by confining cubic CoSe2 nanoparticles to three‐dimensional (3D) porous MOFs‐derived nitrogen‐doped carbon (NC) and one‐dimensional (1D) N‐doped carbon nanofibers (NCNFs) through a facile encapsulate strategy. The 1D/3D continuous network structure contributes to the improvement of specific surface area and electronic conductivity, while the strong synergistic effect between CoSe2 sites and Co‐Nx‐C sites can effectively enhance electron/mass transfer and reduce the diffusion resistance. The as‐constructed CoSe2@NC@NCNFs catalyst exhibit high catalytic activity and stability toward ORR/OER with a high half‐wave potential of 0.80 V (vs. RHE) in ORR and a low overpotential of 280 mV at 10 mA cm−2 in OER. More encouragingly, the rechargeable ZABs with CoSe2@NC@NCNFs cathode deliver high peak power densities (126.8 mW cm−2), large specific capacities (763.1 mA h g−1), and robust charge‐discharge cycling stability over 240 cycles. This study provides a facile strategy for designing efficient bifunctional catalysts for rechargeable energy conversion applications.This article is protected by copyright. All rights reserved.