Recently environmental-friendly and recyclable solid catalysts for the production of fine chemicals are eagerly required. The catalytic activity of alkali metal-exchanged Al-containing KIT-1(Na-AlKIT-1, K-AlKIT-1, and Rb-AlKIT-1) as a base catalyst for organic reaction, especially Knoevenagal reaction was studied. The heterogeneous catalytic Knoevenagel reaction using the alkali-containing AlKIT-1 as the catalyst such as AlKIT-1, Na-AlKIT-1, K-AlKIT-1, and Rb-AlKIT-1, is performed with the solvent or without solvent. The solvent-free system gives promising results. Among them, Rb-AlKIT-1 seems the best catalyst for this reaction.