This research focuses on improving the characteristics of recycled concrete and utilizing solid waste resources through the combination of industrial waste pre-impregnation and the carbonation process. A novel pre-impregnation–carbonation aggregate method is proposed to increase the content of carbonatable components in the surface-bonded mortar of recycled coarse aggregate by pre-impregnating it with carbide slag slurry (CSS). This approach enhances the subsequent carbonation effect and thus the properties of recycled aggregates. The experimental results showed that the method significantly improved the water absorption, crushing value, and apparent density of the recycled aggregate. Additionally, it enhanced the compressive strength, split tensile strength, and flexural strength of the recycled concrete produced using the aggregate improved by this method. Microanalysis revealed that CO₂ reacts with calcium hydroxide and hydrated calcium silicate (C-S-H) to produce calcite-type calcium carbonate and amorphous silica gel. These reaction products fill microcracks and pores on the aggregate and densify the aggregate–paste interfacial transition zone (ITZ), thereby improving the properties of recycled concrete. This study presents a practical approach for the high-value utilization of construction waste and the production of low-carbon building materials by enhancing the quality of recycled concrete. Additionally, carbon sequestration demonstrates broad promise for engineering applications.