Concrete structures provided with steel bars may undergo deterioration due to fatigue and corrosion, which leads to an increase in repair and maintenance costs. An innovative approach to eliminating these drawbacks lies in the utilisation of glass-fibre-reinforced polymer (GFRP) sheets as reinforcement in concrete structures instead of steel bars. This article relates to the investigation of the flexural behaviour of ordinary portland cement (OPC) concrete slabs and high-volume fly ash (HVFA) concrete slabs reinforced with bi-directional GFRP sheets. Slab specimens were cast with 60% fly ash as a replacement for cement and provided with a 1 mm-thick GFRP sheet in 2, 3 and 4 layers. The flexural behaviour of slabs reinforced with GFRP sheets was compared with that of the slabs reinforced with steel bars. Experiment results such as cracking behaviour, failure modes and load–deflection, load–strain and moment–curvature relationships of the slab specimens are presented. Subsequently, the nonlinear finite-element method (NLFEM) using ANSYS Workbench 2022-R1 was carried out and compared with the experimental results. The results obtained from the numerical investigation correlated with the experimental results. The experimental investigation showed that the HVFA concrete slabs reinforced with GFRP sheet provided a better alternative compared to the steel reinforcement, which led to sustainable construction.