Materials for the conservation of cultural heritage must meet specific demands, such as high durability, service life, and compatibility with other materials used in the original building structures. Due to their low permeability to water and water vapor and their high rigidity, the use of Portland cement (PC) mortars, despite their high mechanical resistance and durability, does not represent an appropriate solution for the repair of historic masonry and structures. Their incompatibility with the original materials used in the past, often on a lime basis, is therefore a serious deficiency for their application. On the other hand, lime-based mortars, compared to PC-based materials, are more susceptible to mechanical stress, but they possess high porosity, a high water vapor transmission rate, and moderate liquid water transport. This study aims at the development of two types of lime-based mortars, calcium lime (CL) and hydraulic lime (HL). The modification of mortars was conducted with a carbon-based nanoadditive and graphene nanoplatelets (GNs) in three dosages: 0.1%, 0.3%, and 0.5% of the binder weight. The enhancement of CL mortars by GNs greatly increased mechanical strength and affected heat transport characteristics, while other characteristics such as porosity, water absorption, and drying rate remained almost similar. The application of GNs to HL not only enhanced the strength of mortars but also decreased their porosity, influenced pore size distribution, and other dependent characteristics. It can be concluded that the use of graphene nanoplatelets as an additive of lime-based composites can be considered a promising method to reinforce and functionalize these composite materials. The improved mechanical resistance while maintaining other properties may be favorable in view of the increasing requirements of building materials and may prolong the life span of building constructions.