Purified terephthalic acid (PTA) is widely used as a chemical raw material, with its production process resulting in significant compounds that generate a substantial amount of sludge waste annually. These compounds are known to possess active hydrogen. Utilizing this property, a novel approach for the treatment of PTA sludge waste was developed for its modification and re-use. This study focuses on the preparation of epoxy curing agents using PTA sludge-tank material. The modification of PTA sludge-tank material is achieved by using the one-pot method to investigate the toughening effect of home-made curing agents on epoxy resins and compare them with commercially available curing agents, and to analyze the mechanism of the structure of the curing agent on the material. The results showed that while the tensile strength of the experimental group was generally lower than that of the control group, the impact strength was significantly higher. Additionally, the hardness and tensile strength of the materials gradually decreased with an increase of the amount of hardener, while the elongation at break and impact strength increased. Notably, at a hardener amount of 35%, the elongation at break increased by 3.89%, and the tensile strength and impact strength reached 10.13 MPa and 42.86 kJ m−2, respectively, demonstrating excellent toughness and strength characteristics. These findings testified the feasibility of modifying PTA sludge waste to prepare an epoxy toughening curing agent is not only feasible, but also significantly enhances the material’s toughness.