In summary, even though XRD results indicated that the ZrHEDP samples were amorphous states and no clear peaks for the layer-by-layer structure, the peaks for Zr-Zr distance were detected, which is more critical than the layer-by-layer structure to retain the -PO3H2 close. Furthermore, ICP-AES and NMR results suggested a larger amount of -PO3H2 as P/Zr increases. Furthermore, as the essential insights, FT-IR and DSC results identified the interaction of -PO3H2 in close proximity. These results indicate that ZrHEDP with high P/Zr has a lot of -PO3H2 at a close distance to interact with each other.