The work described in this paper has been performed to determine the potential use of meta-illite (KyAl4(Si8-y) O20(OH)4) calcined clay (MCC) as a supplementary cementitious material (SCM) in a binary Portland cement (PC) for high-performance concrete (HPC) production. To obtain the properties of the cementitious materials, the chemical composition, mineral phases, morphology, calcination efficiency and physical properties were quantitatively analysed using the advanced techniques of X-ray fluorescence (XRF), scanning electron microscopy/energy dispersive X-ray (SEM/EDX), X-ray diffraction (XRD), Fourier transform infrared/attenuated total reflection (FTIR/ATR), thermogravimetric analysis (TGA), laser particle sizing and Brunauer–Emmett–Teller (BET) nitrogen absorption method. The MCC’s effect on the workability and mechanical properties (compressive, splitting tensile and flexural strengths) and microstructure (morphology and crystalline phases) of hardened MCC-based HPCs were determined. The XRF result shows that the oxide composition of MCC confirmed the pozzolanic material requirements with recorded high useful oxides content. At the same time, the SEM image presents particles of broad, solid masses with a wider surface area of irregular shape. The XRD results show that the MCC was majorly an illite-based clay mineral calcined at a maximum temperature of 650 °C, as revealed by the TGA. The MCC addition increases the slump flow of HPCs at 5–15% cement replacement. The MCC incorporation at 10% cement replacement best improved the porosity of HPCs at a later age resulting in increased mechanical and microstructural properties of tested samples. Therefore, it is recommended that MCC addition within 10% cement replacement be adopted for low W/B Class I HPC at no deleterious results on mechanical and microstructural properties of the concrete.