Calcium carbide slag and silica fume was used as a cement replacement material, combined with excavated soil and EPS (expanded polystyrene) particles, to develop a new green and low-carbon lightweight fluid solidified soil (LFSS). Focusing on the performance regulation of LFSS, this study adopted the paste volume ratio (PV, defined as the volume ratio of paste to total mixture) and the water–binder ratio (w/b) to systematically construct a mix ratio design system and proposed EPS particle interface modification and shell formation technology to improve the weak interface bonding between EPS and the matrix. Firstly, based on the paste volume method, the effects of PV and w/b on the flowability and strength of LFSS were analyzed, and a linear correlation model between the water–solid volume ratio and flowability, as well as a quadratic function prediction model for 28-day strength, was established. Secondly, the “core–shell structure” of EPS particles was constructed by combining EVA (ethylene-vinyl acetate) modification with the coating of calcium carbide slag–silica fume paste. Considering the influence of the coating method, w/b, and material mass ratio on interface bonding comprehensively, the optimal process parameters were determined to achieve the interface reinforcement of EPS particle. The results showed that the water–solid volume ratio was significantly linearly correlated with the flowability of LFSS. PV and w/b respectively controlled the framework formation and pore structure evolution of LFSS, with optimal overall performance at PV = 0.55 and w/b = 2.5. The modification shell formation significantly reduced the shell loss rate of EPS particles and increased the 28-day compressive strength of LFSS by 21.7%. SEM (scanning electron microscope) and EDS (energy-dispersive spectroscopy) analysis further revealed that the shell-formation technique promoted the densification of the interface transition zone, enhanced the deposition of hydration products, and strengthened the synergistic effect of Na and Ca elements, thereby significantly improving interface bonding and overall structural stability. This study established a “mix ratio optimization-modification and shell formation” dual-regulation mechanism, providing an effective technical approach and theoretical basis for the engineering application of calcium carbide slag–silica fume-based LFSS.