Recycled concrete fines (RCFs) have the potential to serve as a supplementary cementitious material (SCM) after carbonation. Traditionally, carbonation of RCFs results in calcium carbonate primarily in the form of calcite, which significantly limits the development of RCFs as an SCM. In this research, a wet grinding carbonation (WGC) technique was introduced to enhance the reactivity of RCFs. The research indicates that RCFs after WGC exhibit a finer particle size and a larger specific surface area. The carbonation products include calcite with smaller grains, metastable calcium carbonate, and nanoscale silica gel and Al-Si gel. When RCF-WGC is used as an SCM in ordinary Portland cement (OPC), it significantly promotes the hydration of the cement paste, as evidenced by the advancement and increased intensity of the exothermic peaks of aluminates and silicates. RCF-WGC can significantly enhance the compressive strength of hydrated samples, particularly at early ages. Specifically, at a curing age of 1 day, the compressive strength of WGC5, WGC10, and WGC20 samples increased by 9.9%, 22.5%, and 7.7%, respectively, compared to the Ref sample (0% RCF-WGC). At a curing age of 3 days, the compressive strength of the WGC5, WGC10, and WGC20 samples showed even more significant improvements, increasing by 20.8%, 21.9%, and 11.8%, respectively. The performance enhancement of the WGC samples is attributed to the chemical reactions involving nanoscale silica gel, Al-Si gel, and calcium carbonate in the RCFs. When RCF-WGC is used as an SCM to replace 5%, 10%, and 20% of cement, it can reduce carbon emissions by 27.5 kg/t, 55 kg/t, and 110 kg/t, respectively. Large-scale application of RCFs as a high-value SCM can significantly reduce the life-cycle carbon emissions of the cement industry, contributing to the achievement of carbon peaking in China’s cement sector.