Bicontinuous, thermosensitive, L-3-phase silica nanocomposites are prepared by self-assembly of silicified L-3-phase silicates and L-3-phase silicates integrated with thermoresponsive poly(N-isopropylacryl amide) (PNIPAm; see Figure). In the L-3-PNIPAm material, interpenetrating nanoscale networks of silica and polymer gel are formed, with which highly controlled drug delivery is successfully demonstrated.