The preparation of healable and recyclable polymers with balanced strength and ductility remained challenging in polymer science. Herein, a fully biobased two-functional imine modifier (2VP) was synthesized through a Schiff base reaction between vanillin and a branched diamine (Priamine 1074) in one pot without solvent. Imine vitrimers with a high biomass content (about 70%) were prepared by reacting 2VP with isocyanates, of which hexamethylene diisocyanate trimer (HDI-T) acted as a crosslinker and isophorone diisocyanate (IPDI) acted as a chain extender, at a moderate temperature (80 °C). The rigid aromatic vanillin and flexible branched diamine endowed the imine vitrimers with moderate strength and excellent ductility; their optimal tensile strength and elongation at break were 38.7 ± 1.91 MPa and 347.6 ± 20.6%, respectively. The imine vitrimers exhibited fast stress relaxation at temperatures between 80 and 110 °C, indicating a rapid network rearrangement through imine metathesis. Thus, the imine vitrimers were facilely healed and recycled at 80 °C with high efficiency. The extension of the molecular chains of the imine vitrimers lowered tensile strength, storage modulus, and T_g but increased ductility, thermal stability, and healing and recycling efficiency.