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The compounds are isostructural and crystallise in space group <jats:italic>P<\/jats:italic><jats:sub>\u22121<\/jats:sub> with the following parameters: NaCa(PO<jats:sub>3<\/jats:sub>)<jats:sub>3<\/jats:sub>, <jats:italic>a<\/jats:italic> = 6.711 \u00c5, <jats:italic>b<\/jats:italic> = 6.934 \u00c5, <jats:italic>c<\/jats:italic> = 7.619 \u00c5, \u03b1 = 83.44\u00b0 , \u03b2 = 81.41\u00b0 , \u03b3 = 82.80\u00b0 ; NaSr(PO<jats:sub>3<\/jats:sub>)<jats:sub>3<\/jats:sub><jats:italic>a<\/jats:italic> = 6.805 \u00c5, <jats:italic>b<\/jats:italic> = 7.133 \u00c5, <jats:italic>c<\/jats:italic> = 7.720 \u00c5 and \u03b1 = 83.71\u00b0 , \u03b2 = 80.48\u00b0 , \u03b3 = 82.87\u00b0 . Both structures contain anionic metaphosphate chains of (PO<jats:sub>3<\/jats:sub>)<jats:sub><jats:italic>n<\/jats:italic><\/jats:sub><jats:sup><jats:italic>n<\/jats:italic><\/jats:sup> with ionic contacts to Na<jats:sup>+<\/jats:sup> ions in distorted octahedral sites and Ca<jats:sup>2+<\/jats:sup> (or Sr<jats:sup>2+<\/jats:sup>) in distorted dodecahedral sites. <jats:sup>31<\/jats:sup>P and <jats:sup>23<\/jats:sup>Na NMR are entirely consistent with the crystallographic data and an empirical method for assigning <jats:sup>31<\/jats:sup>P resonances to particular crystallographically unique P atoms is described. 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