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This research investigates the preparation and characterization of new organic–inorganic geopolymeric foams obtained by simultaneously reacting coal fly ash and an alkali silicate solution with polysiloxane oligomers. Foaming was realized in situ using Si⁰ as a blowing agent. Samples with density ranging from 0.3 to 0.7 g/cm³ that show good mechanical properties (with compressive strength up to ≈5 MPa for a density of 0.7 g/cm³) along with thermal performances (λ = 0.145 ± 0.001 W/m·K for the foamed sample with density 0.330 g/cm³) comparable to commercial lightweight materials used in the field of thermal insulation were prepared. Since these foams were obtained by valorizing waste byproducts, they could be considered as low environmental impact materials and, hence, with promising perspectives towards the circular economy.