An efficient synthesis methodology to obtain homogeneous nanosized high-silica Beta zeolites (∼10–20 nm) with high solid yields (above 95%) using simple alkyl-substituted flexible dicationic OSDAs is described. These dicationic OSDAs allow the synthesis of nanosized Beta zeolites with different Si/Al ratios (15–30) in alkaline and fluoride media, resulting in nanocrystalline materials with different physico-chemical properties. These nanosized Beta zeolites show better catalytic behavior towards the industrially-relevant alkylation of benzene with propylene to obtain cumene compared with other commercially available nanosized Beta zeolites.