Growing sustainability concerns have promoted the rapid development of reusable and environmentally friendly thermosetting materials. Herein, a recyclable biobased curing agent (vanillin-based imine curing agent) was produced from vanillin in a single-stage process. However, this curing agent was fully solid and difficult to process, requiring large amounts of solvent during processing. Since the viscosity of 4-methyl-1,3cyclohexendiamine (HTDA) is low, it can be used as a cocuring agent at various amounts to make a viscous liquid curing agent for diglycidyl ether of bisphenol F. The curing behaviors and thermomechanical and mechanical properties of the cured thermosets were evaluated along with their self-healing ability. The results reveal that the viscosity and activation energy of curing are reduced as the weight ratio of HTDA increases, whereas the flexural strength (106−122 MPa), moduli (2365−2587 MPa), and T g values (95−110 °C) increase gradually. Additionally, the heat-resistant temperature (T s ) values (166−162 °C) and char residue at 700 °C (26−10%) of the cured samples continuously decreased. Overall, 40% HDTA containing VH03 showed a suitable viscous form for processing and mechanical and thermal properties. Subsequently, the flexural strength retention and T g were still 80% and 115 °C, respectively, and it also demonstrated absolute solvent resistance at room temperature. The excellent integrated properties clarified that VH03 is favorable for easy processability, recyclability, and sustainable improvement.