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Development of bio-based vitrimers attracted significant attention due to these species’ excellent recyclability and renewability. However, most bio-based vitrimers require high-temperature curation and catalyst use. Herein, room temperature-curable vanillin-based vitrimers were prepared via a catalyst-free route involving a Schiff base reaction and an amino–yne click reaction; the obtained vitrimers exhibited excellent recyclability and high degradability under mild conditions. The chemical structures, mechanical properties, and thermal stability of the obtained crosslinked networks were characterized in detail. These networks displayed good malleability performance, reflected by values for the glass transition temperature of 55–62 °C, tensile strength of 13–15 MPa, and elongation at break of 77–98%. Notably, the vitrimer networks exhibited recyclability due to the multifunction dynamic exchange reactions of Schiff base network and enamine–one network (amino–yne click reaction). More interestingly, these vitrimers could be completely degraded in mild organic acid, organic base, and amine solutions.