The paper presented herein investigates the effects of using supplementary cementitious materials (SCMs) in quaternary mixtures on the compressive strength and splitting tensile strength of plain concrete. In addition, environmental benefits resulting from the proposed solutions were analysed. A total of four concrete mixtures were designed, having a constant water/binder ratio of 0.4 and total binder content of 352 kg/m3. The control mixture only contained ordinary Portland cement (OPC) as binder, whereas others incorporated quaternary mixtures of: OPC, fly ash (FA), silica fume (SF), and nanosilica (nS). Based on the obtained test results, it was found that concretes made on quaternary binders containing nanoadditives have very favorable mechanical parameters. The quaternary concrete containing: 80% OPC, 5% FA, 10% SF, and 5% nS have shown the best results in terms of good compressive strength and splitting tensile strength, whereas the worst mechanical parameters were characterized by concrete with more content of FA additive in the concrete mix, i.e., 15%. Moreover, the results of compressive strength and splitting tensile strength are qualitatively convergent. Furthermore, reducing the amount of OPC in the composition of the concrete mix in quaternary concretes causes environmental benefits associated with the reduction of: raw materials that are required for burning clinker, electricity, and heat energy in the production of cement.