This study investigates the valorization of dredged sludge as a sustainable subgrade fill material through stabilization with a nano-calcium carbonate–cement composite. Unconfined compressive strength (UCS) tests were systematically conducted to determine the optimal dosage of nano-CaCO₃ as a supplementary additive at a fixed cement content of 8% by dry soil mass. Scanning electron microscopy (SEM), X-ray diffraction (XRD), and quantitative pore structure analysis were employed to elucidate the underlying solidification mechanisms. The results demonstrate that the addition of 2% nano-CaCO₃ yields the highest 28-day UCS of 721 kPa, representing a statistically significant 21% improvement over the cement-only reference (596 kPa) and a more than threefold increase relative to untreated sludge (213 kPa). Conversely, increasing the nano-CaCO₃ dosage to 2.5% leads to a significant strength reduction, attributed to nanoparticle agglomeration and hindered cement hydration. Microstructural characterization reveals that the optimal nano-CaCO₃ dosage accelerates early-age hydration through a nucleation effect, promotes the consumption of portlandite, and enhances the formation of calcium silicate hydrate (C–S–H) gel. Semi-quantitative XRD analysis further confirms the conversion of less stable monosulfate (AFm-SO₄) into stable monocarboaluminate (AFm-CO₃) phases. These synergistic mechanisms—nucleation, physical pore filling, and chemical reaction—result in a densified matrix with a refined pore structure, reduced total porosity, and a more homogeneous pore-size distribution. The findings provide a robust theoretical basis for the resource-oriented utilization of dredged sludge and the design of low-carbon composite stabilizers for soft soil treatment.