In this study, improved nanoporous zeolites for use in post-combustion carbon capture have been synthesised from industrial-grade biomass combustion fly ash generated in one of the largest biomass combustion power plants in the UK. The method of nanoporous zeolite synthesis follows an alkaline fusion-assisted hydrothermal procedure. The nanoporous zeolites have been characterised by scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS), X-ray diffraction (XRD) and Fourier-transform infrared spectroscopy (FTIR). The presence of two crystalline structures, Faujasite and Linde Type A has been confirmed by the characterisation results. The CO2 adsorption investigations were conducted via thermogravimetric analysis (TGA) to estimate the uptake capacity of the prepared adsorbents. TGA studies suggest that the improved nanoporous adsorbent, evaluated under 100 mol% CO2 at atmospheric pressure, has an equilibrium capacity of over 1.6 mmolCO2/g at 50 °C, a two-fold increase from our previous study with a crystalline structure confirmed by XRD.