Defect　engineering　is　one　of　the　effective　ways　to　improve　the　electrochemical　property　of　electrode　materials　for　lithium-ion　batteries　(LIB).　Herein,　an　organic　functional　molecule　of　pphenylenediamine　is　embedded　into　two-dimensional　(2D)　layered　TiO2　as　the　electrode　for　LIB.　Then,　the　2D　carbon/TiO2　composites　with　the　tuning　defects　are　prepared　by　precise　control　of　the　polymerization　and　carbothermal　atmospheres.　Low　valence　titanium　in　metal　oxide　and　nitrogendoped　carbon　nanosheets　can　be　obtained　in　the　carbon/TiO2　composite　under　a　carbonization　treatment　atmosphere　of　N2　/H2　gas,　which　can　not　only　increase　the　electronic　conductivity　of　the　material　but　also　provide　sufficient　electrochemical　active　sites,　thus　producing　an　excellent　rate　capability　and　long-term　cycle　stability.　The　prepared　composite　can　provide　a　high　capacity　of　396.0　mAh　g−1　at　a　current　density　of　0.1　A　g−1　with　a　high　capacitive　capacity　ratio.　Moreover,　a　high　specific　capacity　of　80.0　mAh　g−1　with　retention　rate　of　85%　remains　after　10,000　cycles　at　3.0　A　g−1　as　well　as　the　Coulomb　efficiency　close　to　100%.　The　good　rate-capability　and　cycle-sustainability　of　the　layered　materials　are　ascribed　to　the　increase　of　conductivity,　the　lithium-ion　transport　channel,　and　interfacial　capacitance　due　to　the　multi-defect　sites　in　the　layered　composite.　©　2022　by　the　authors.　Licensee　MDPI,　Basel,　Switzerland.