As　a　key　factor　for　fast-charging　lithium-ion　batteries　(LIBs),　high-rate　anode　materials　that　can　recharge　in　a　few　minutes　have　aroused　increasing　attention.　However,　high-rate　performance　is　always　accompanied　by　low　theoretical　capacities,　such　as　the　widely　known　high-rate　electrode　of　Li4Ti5O12　(175　mA　h　g-1),　which　severely　limits　its　large-scale　implementation　in　the　development　of　high　power　density　LIBs.　Here,　we　report　a　modified　close-spaced　thermal　evaporation　process　to　deposit　3D-structured　Sb2Se3　films　(3D-SSF)　with　tunable　morphology　as　an　additive-free　anode　for　LIBs.　After　a　high-rate　activation　process,　3D-SSF　exhibits　a　flatter　discharge　plateau　than　the　reported　results　and　could　deliver　a　high　capacity　of　471　mA　h　g-1　at　an　ultrahigh　current　density　of　21　440　mA　g-1,　which　is　superior　to　the　widely　known　high-rate　Li4Ti5O12　anode　(over　150　mA　h　g-1　at　8750　mA　g-1).　Moreover,　we　reveal　a　current-regulated　Li-ion　storage　mechanism　where　3D-SFF　undergoes　a　synergistic　conversion　and　alloying　reaction　at　low　current　densities,　while　an　alloying　reaction-dominated　process　at　high　rates.　Beyond　that,　full　batteries　with　excellent　rate　performance　were　successfully　assembled　by　pairing　with　homemade　LiFePO4　(LFP)　as　the　cathode.　This　journal　is　©　The　Royal　Society　of　Chemistry.