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The cost-efficient and plentiful Na and K resources motivate the research on ideal electrodes for sodium-ion batteries (SIBs) and potassium-ion batteries (PIBs). Here, MoSe2nanosheets perpendicularly anchored on reduced graphene oxide (rGO) are studied as an electrode for SIBs and PIBs. Not only does the graphene network serves as a nucleation substrate for suppressing the agglomeration of MoSe2nanosheets to eliminate the electrode fracture but also facilitates the electrochemical kinetics process and provides a buffer zone to tolerate the large strain. An expanded interplanar spacing of 7.9 Å is conducive to fast alkaline ion diffusion, and the formed chemical bondings (C–Mo and C–O–Mo) promote the structure integrity and the charge transfer kinetics. Consequently, MoSe2@5%rGO exhibits a reversible specific capacity of 458.3 mAh·g–1at 100 mA·g–1, great cyclability with a retention of 383.6 mAh·g–1over 50 cycles, and excellent rate capability (251.3 mAh·g–1at 5 A·g–1) for SIBs. For PIBs, a high first specific capacity of 365.5 mAh·g–1at 100 mA·g–1with a low capacity fading of 51.5 mAh·g–1upon 50 cycles and satisfactory rate property are acquired for MoSe2@10%rGO composite. Ex situmeasurements validate that the discharge products are Na2Se for SIBs and K5Se3for PIBs, and robust chemical bonds boost the structure stability for Na- and K-ion storage. The full batteries are successfully fabricated to verify the practical feasibility of MoSe2@5%rGO composite.