Layered hydrazinium titanate (LHT-9) has been synthesized by reflux and microwave routes and evaluated for its potential application for sequestration of radionuclides from nuclear waste. Synthesized materials have been characterized using X-ray diffraction, scanning electron microscopy, X-ray absorption spectroscopy and uptake of radionuclides. The LHT-9 obtained by the microwave route appears more ordered than that obtained using the reflux process. However, both are comprised of TiO₆ octahedra. Post loading of species such as Sr, the octahedral ordering within the layers remains intact. Considering the uptake behaviour and the possibility of scale-up, LHT-9 synthesis using the microwave route may provide advantages in nuclear waste treatment applications.