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　p-phenylenediamine　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　nitrogen-doped　carbon　nanosheets　can　be　obtained　in　the　carbon/TiO2　composite　under　a　carbonization　treatment　atmosphere　of　N-2/H-2　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.