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Highlights Extrinsic doping is proposed as a novel route to enhance the intrinsic properties of the two-dimensional oxidized Si nanosheet (namely, siloxene) anode for Li-ion batteries. Fabrication of P-doped n-type siloxene is revealed to be possible through selective nucleophilic substitution of Si atoms in siloxene with P atoms. Due to boosted charge transport kinetics, n-type siloxene (6.7 × 1019 P atoms cm-3) exhibits the excellent storage performance (594 mAh g-1 after 500 cycles) even at 2000 mA g-1.