The use of hybrid organic/inorganic materials for self-healing concrete is an alternative to minimize the negative environmental impacts of cement demand to repair and rehabilitate concrete structures and design innovative construction materials for practical application in the field. However, the performance of self-healing concrete, with additions of different chemical natures, like organic, inorganic, and biological materials, needs to be assessed to determine its effect on fresh and hardened concrete characteristics like workability and mechanical resistance. Moreover, self-healing efficiency is a determinant parameter that should be accomplished for the potential use of these materials. Thus, self-healing concrete must present functional self-healing features to overcome microcracking and improve its intrinsic characteristics. Within autonomous self-healing technologies, microcapsule-based systems offer advantages due to their easy incorporation into the cementitious matrix and their compositional versatility. Many studies have been done using silica-shell with organic and inorganic cores. Also, silicate-core was encapsulated with different organic shells. However, its implementation is ineffective, and reductions in strength and fluency are additional obstacles to their practical application. In this research, microcapsules were produced with Silicate-based (MC-SS) and Biopolymer/Silicate-based (MC-SS-St) cores, covered by a silica-shell, on a laboratory scale using renewable raw materials and soft chemistry synthesis process. The influence of the produced microcapsules in the cementitious mixtures and the self-healing efficiency were evaluated for additions of 2.5, 5.0, and 7.5 wt% in cement replacement. Results indicated a homogeneous distribution of the microcapsules, no influence on fresh properties, and the recovery of mechanical strength and transport properties through an autonomous self-healing mechanism. The evaluated materials presented a suitable performance for developing low carbon footprint and functional self-healing construction materials, which can be improved for higher dosages and scaled to concrete mixtures.