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Evidence of the association of magnesium (Mg) with arterial stiffness has so far been conflicting. The interplay between hypertension and elevated body mass index (BMI), with hypomagnesemia, instead, has been described in the literature in a more consistent way. Our study aims at revisiting the correlations between blood Mg levels and hemodynamic and body composition parameters in the general population, exploring the sensitivity profile of ionized Mg (Ion-Mg) compared to total Mg (Tot-Mg). We collected data from 755 subjects randomly chosen from a Swiss population previously described and stratified our sample into four equivalent classes according to ionized (whole blood) and total (serum) magnesium. After correcting for age, statistically significant differences emerged between: (i) Tot-Mg ≤ 0.70 and 0.81 ≤ Tot-Mg ≤ 0.90 for cf-PWV (p = 0.039); (ii) Tot-Mg ≤ 0.70 and Tot-Mg ≥ 0.91 for o-PWV (p = 0.046). We also found a statistically significant difference among groups of Ion-Mg values for the 24 h extremes of systolic blood pressure (p = 0.048) and among groups of Tot-Mg for BMI (p = 0.050). Females showed significantly lower levels of total magnesium (p = 0.035) and ionized magnesium (p < 0.001) than males. The overall agreement between magnesium analysis methods was 64% (95%CI: 60.8−67.7%). Our results confirm that Ion-Mg compared with Tot-Mg offers a different profile in detecting both correlations with hemodynamic and body composition parameters and dysmagnesemias. Lower levels of magnesium were associated with worse arterial aging parameters, larger 24 h blood pressure excursions, and higher BMI. Ion-Mg was superior in detecting the correlation with blood pressure only. Considering Ion-Mg as a more specific marker of the magnesium status, and the partially contradictory results of our explorative cross-sectional study, to avoid confounding factors and misinterpretations, ionized magnesium should be used as reference in future studies.