MXene　species　have　emerged　as　a　class　of　compelling　electrode　materials　in　the　field　of　capacitive　deionization　(CDI).　However,　as　an　excellent　member　of　the　MXene　family,　the　Nb4C3Tx　has　not　received　much　attention　in　terms　of　CDI.　Herein,　we　have　not　only　established　the　feasibility　of　Nb4C3Tx　as　a　potential　desalination　electrode　materiel　but　also　proposed　a　wrinkle-engineering　strategy　that　can　effectively　improve　the　CDI　performance　of　Nb4C3Tx　freestanding　membranes.　Specifically,　the　introduction　of　wrinkles　on　Nb4C3Tx　nanosheets　contributes　to　optimizing　the　interlayer　space,　accessibility,　conductivity,　stability,　and　CDI　performance　of　the　assembled　membranes.　In　particular,　the　optimized　wrinkled　Nb4C3Tx　membranes　can　achieve　an　ultrahigh　desalination　capacity　of　similar　to　188.2　mg　g(-1)　at　1.6　V　accompanied　by　a　fast　adsorption　rate　of　similar　to　12.6mg　g(-1)　min(-1),　showing　great　competitiveness　with　other　MXene　individual　electrodes.　In　addition,　the　as-designed　electrodes　also　exhibit　superior　cycle　desalination　stability　as　well　as　good　applicability　to　different　salts　(such　as　LiCl,　KCl,　CaCl2,　and　MgCl2).　This　work　both　extends　the　MXene　material　applicable　to　CDI　and　offers　an　effective　solution　for　improving　the　properties　of　Nb4C3Tx-MXene　lamellar　membrane　electrodes,　opening　up　enormous　opportunities　for　the　use　of　such　MXene　species　in　the　field　of　electrochemical　desalination.