Capacitive　deionization　(CDI)　based　on　the　theory　of　a　double　electric　layer　has　received　much　attention　in　the　past　two　decades　as　a　highly　promising　desalination　technology,　and　carbon　nanospheres　are　considered　promising　carbon-based　electrode　materials　for　CDI,　which　have　been　investigated　by　a　large　number　of　researchers.　However,　the　isolation　between　the　spheres　greatly　increases　the　contact　resistance,　limiting　their　application　in　CDI.　To　understand　the　effect　of　structure　on　the　performance　of　CDI　and　to　obtain　a　better　CDI　performance,　solid　carbon　spheres　and　monodisperse　hollow　carbon　spheres　were　prepared　and　compared　with　interconnected　hollow　carbon　spheres　(IHCSs).　The　resulting　IHCSs,　with　their　unique　cavity　structure　and　interconnected　carbon　walls,　exhibited　superior　electrochemical　performance　and　electrosorption　capacity.　In　addition,　we　improved　the　electrical　conductivity,　surface　wettability,　and　adsorption　properties　of　the　carbon　nanospheres　by　incorporating　nitrogen　doping.　By　adjusting　the　amount　of　nitrogen　functional　groups　in　the　carbon　nanosphere　precursors,　we　produced　interconnected　hollow　carbon　nanospheres　with　similar　structures　(particle　size,　specific　surface　area,　and　porosity)　but　different　nitrogen　contents　and　investigated　the　effects　of　different　nitrogen　contents　on　the　CDI　properties　of　hollow　carbon　nanospheres.　The　results　indicated　that　interconnected　hollow　carbon　nanospheres　with　a　high　nitrogen　content　(designated　as　NFs-2)　demonstrated　the　best　CDI　performance,　achieving　an　electrochemical　adsorption　capacity　of　20.43　mg　g-1　in　a　NaCl　solution　with　a　concentration　of　500　mg　L-1.　Additionally,　NFs-2　exhibited　the　largest　specific　surface　area　of　728　m2　g-1.　Furthermore,　NFs-2　displayed　excellent　cycle　stability　in　a　desalination　cycle　using　a　100　mg　L-1　NaCl　solution,　retaining　up　to　97.17%　of　its　initial　desalination　capacity　after　25　sorption-desorption　cycles.　These　findings　highlight　the　promising　applications　of　NFs-2　in　CDI　technology.　©　2023　American　Chemical　Society