Fibre-reinforced cementitious materials represent one of the most significant developments in the field of concrete technology of the last decades. The improved performance of this new class of materials (in terms of workability, compressive strength, flexural/tensile behaviour and/or durability) allows rethinking several of the existing structural solutions. This paper describes research on high-performance fibre reinforced concrete (HPFRC) to be used at the slab-column connection zones of flat slabs, in order to improve its punching shear resistance. Design of Experiments (DoE) approach was used to design HPFRC paste and aggregate particle phases. As such, a central composite design was carried out to mathematically model the influence of mixture parameters and their coupled effects on deformability, viscosity and compressive strength. After that, a numerical optimization technique was applied to the derived models to select the best mixture, which simultaneously, maximizes aggregates content and allows achieving a compressive strength of 90–120 MPa, while maintaining self-compactability (SF1 + VS2), incorporating 1% steel fibres content.