Titanium-based　anode　materials　are　attracting　considerable　attention　for　use　in　high-performance　lithium-ion　batteries,　but　the　compromised　energy　density　caused　by　high　voltage　plateaus　and　unsatisfactory　capacities　severely　retards　their　practical　applications.　Herein,　a　molten-salt　synthesis　of　Li(2)TiSiO(5)crystalline　platelets　and　a　subsequent　selective　facet　modification　by　in　situ　growth　of　TiO(2)nanocrystal　frames　are　facilely　achieved.　The　discharge　voltage　plateau　at　around　0.5　V　renders　the　Li(2)TiSiO(5)anode　safe　compared　with　graphite　and　confers　a　high　energy　density　compared　with　zero-strain　Li(4)Ti(5)O(12)anode.　With　the　optimized　size,　structure,　and　content　of　modified　TiO(2)nanocrystals　associated　with　the　exposed　(001)　plane　of　Li2TiSiO5,　the　Li2TiSiO5-based　anodes　can　deliver　a　capacity　of　above　300　mAh　g(-1),　enhanced　rate　performance,　and　a　capacity　retention　of　66%　after　10　000　cycles.　In　situ　X-ray　diffraction　and　ex　situ　transmission　electron　microscopy　have　demonstrated　the　structural　stability　of　the　anodes　upon　charge/discharge.　Further　theoretical　calculation　reveals　3D　migration　paths　of　Li(+)ions　in　Li2TiSiO5.　The　selective　modification　of　in　situ　grown　TiO(2)nanocrystals　on　certain　facets　of　crystallites　opens　a　new　door　for　the　development　of　electrode　materials　possessing　superior　electrochemical　properties.