This study explored the viability of synthesising nanolime at ambient temperature by raising calcium solubility through the formation of complexes with dissolved sugars. Micro-Raman findings confirmed the formation of nanolime particles whilst the percentage of Ca(OH)2 formed, observed to vary with synthesis conditions, was calculated with thermogravimetry. Nanoparticles were synthesised most productively (77%) in a 5% sugary solution at a temperature of 25 °C and a 4 h reaction time. The hexagonal nanoparticles synthesised ranged in size from 200 to 25 nm. Portlandite formation is related to calcium complex formation with less mannitol that sucrose needed to form similar NPs of Ca(OH)2. The sugary media also favoured the formation of amorphous calcium carbonate.