Natural hydraulic lime-based grouts are often used in the structural consolidation of old stone masonry walls, mainly to re-establish the monolithic behaviour of masonry constructions. To ensure an adequate grouting operation, it is essential to have good fresh and hardened grout properties. The motivation of the present study was to examine the fresh and hardened properties of natural hydraulic lime grouts with nano-silica (NS) and silica fume (SF). The contribution of these materials and the dosage of a high range water reducer admixture (HRWR) were investigated on the rheological properties, water capillarity, open porosity and mechanical strength of injection grouts. The effects on rheology were analysed through plastic viscosity and yield stress. The results indicated that, even for reduced NS content, an increase in plastic viscosity and yield stress occurred, which required a higher HRWR content in order to not compromise the grout’s rheological performance. The results also showed that, when NS and SF were combined, a beneficial joint effect occurred, resulting in a substantial and positive change on the mechanical strength and microstructure of the hardened injection grouts. Taguchi’s method was used to optimize the grout’s formulation and to fulfil the required performance concerning the fresh and hardened state.