The polyoxometalates, or POMs (clusters comprising at least two metal and many oxygen atoms), have recently gained significant interest, owing to their versatile architecture and especially catalytic activities. Due to their high catalytic activity but low surface area, there is always a demand for making high-surface-area POMs, particularly high-surface-area Keggins. Our present work demonstrates the 'gluing' of the anionic phosphomolybdate Keggin on gibbsite nanoplatelets with a residual positive charge to form large-surface-area composites. The resulting composite reported here has been characterized using TEM imaging, EDX/TEM (elemental) analysis, FTIR spectroscopy, potentiometric titrations, electrophoretic mobility determination, and XRD. The composite reported here could be useful in catalysis.