Both　environmental　and　economic　factors　have　driven　the　development　of　degradable　resin　for　carbon　fiber　(CF)　recycling　under　mild　conditions.　However,　the　vast　majority　of　thermosetting　materials　are　difficult　to　recycle.　This　paper　presents　bio-based　polyimine　vitrimers　to　fully　recycle　the　CF.　The　effect　of　vitrimers　fine　structures　on　the　thermal,　mechanical,　solvent　resistance,　and　degradation　properties　is　carefully　investigated.　The　tensile　strength　at　break　and　Young＇s　Modulus　of　pure　polyimine　vitrimers　reach　≈80.3 MPa　and　2.89 GPa.　Importantly,　the　mechanical　property　of　isophoronediamine-based　polyimine　vitrimers/two-layers　CF　exhibits　a　slightly　inferior　value　to　that　of　bisphenol　A　epoxy.　Polyimine　vitrimers　are　easily　degradable　under　acid　solution　at　60 °C　for　24 h.　The　surface　morphology　and　chemical　structure　of　CF　are　not　changed　after　recycling.　This　work　on　mildly　degradable　polyimine　vitrimers　from　vanillin　and　readily　recycling　of　CF　is　desirable　for　the　development　of　eco-friendly　CF　composites　and　lignin　functional　materials.　©　2022　Wiley-VCH　GmbH.