Carbon-doped　TiO2　nanomaterials　have　been　successfully　synthesized　via　an　effective　two-step　procedure　involving　hydrothermal　method　and　followed　by　a　low-temperature　calcination　treatment　process,　through　which　a　controllable　amount　of　carbonate-like　species　could　be　incorporated　into　TiO2.　First-principles　calculations　suggest　the　TiO2　doped　with　carbon　in　form　of　carbonate-like　species　can　effectively　extend　the　adsorption　of　the　material　from　ultraviolet　region　to　visible　light.　And　it　is　experimentally　found　that　carbon-doped　TiO2　nanomaterials　exhibit　much　higher　photocatalytic　activity　than　reference　P25　and　TiO2-xNx　catalysts　toward　the　liquid-phase　degradation　of　organic　pollutants　under　visible　light　(420　nm　＜　＜　800　nm)　irradiation.　The　presence　of　synergic　effect　between　carbonate-like　doping　and　anatase　TiO2　is　believed　to　play　an　essential　role　in　affecting　the　photocatalytic　reactivity,　and　the　response　to　the　visible　light　is　ascribed　to　the　narrowed　band　gap　energy　controlled　by　carbon　doping.　Moreover,　the　roles　of　active　species　in　the　photocatalytic　process　are　compared　using　different　types　of　active　species　scavengers.　Meanwhile,　the　degradation　mechanism　of　the　photocatalysis　is　proposed.　It　is　hoped　that　our　work　could　provide　valuable　information　on　the　design　of　carbonate-like　doped　semiconductor　with　more　excellent　properties　and　set　the　foundation　for　the　further　industrial　application.