The composition of scarbroite, written in the form Al₅(OH)₁₃CO₃·5H₂O, suggests close crystal-chemical relations to gibbsite and to hydrotalcite and kindred minerals. Parametral relations a(S) ≃ 2b(G) and 3b(S) ≃ 5a(G), S = scarbroite, G = gibbsite, are obtained and are consistent with a hydroxy Al layer structure and interlayer carbonate anions and water molecules. Thermal transformations show two discrete hydrated phases with layer spacings near 8.5 and 7.65 Å and a third phase with initial spacing 6.65 Å which decreases progressively to 5.5 Å over the temperature range 100°–250 °C as decomposition proceeds. No clear break is observed between dehydroxylation and decarbonation.