Carbonation is a primary factor driving the continuous improvement of the long-term performance of natural hydraulic lime (NHL). This research systematically examines the impact of accelerated carbonation (3 % CO2) on the carbonation depth, phase composition, microstructure, and compressive strength of hardened natural hydraulic lime (NHL) pastes mixed with different amounts of ground granulated blast furnace slag (GGBFS), termed as S-NHL. The findings show that the hydration reaction products of GGBFS and Ca(OH)2 (CH), such as C3AH10, C4AĈH11, and C-S-H, densify the microstructure of S-NHL, resulting in a decrease in carbonation depth with increasing GGBFS content. Accelerated carbonation (AC) promotes the rapid transformation of a significant quantity of CH into calcite in S-NHL, with the carbonation of CH occurring more readily than the carbonation of hydration reaction products. Throughout the AC process, NHL contains only calcite-type calcium carbonate. In contrast, after 28 days of AC, the carbonation of hydration reaction products such as C3AH10 and C-S-H in S-NHL produces a minor amount of aragonite and vaterite. AC continuously reduces the total pore volume and porosity of S-NHL, but the average pore diameter and most probable pore diameter initially decrease and then slightly increase. AC significantly reduces the large pores in S-NHL, ultimately resulting in pores predominantly composed of capillary pores (50–1000 nm). AC facilitates the development of compressive strength in S-NHL paste, with the increase in compressive strength being positively correlated with its CH content.