This study examined the characteristics of ionized calcium and in vitro calcium bioavailability rate of calcium from four natural sources: shellfish shell, oyster shell, starfish, egg shell. The levels of dissolved calcium and calcium ions increased at different concentrations of natural calcium (up to 8.0% (w/v)). However, there were insignificant differences in the levels of dissolved calcium and calcium ions between samples at calcium concentrations above 8.0% (w/v). In addition, no significant differences were observed (depending on the calcium source and concentration) with an ionization yield of about 90%. The temperature of the solutions also had little influence on the ionization of calcium. The highest calcium ion content was observed when solutions were left to dissolve calcium for 18 hours. The highest in vitro calcium bioavailability rate achieved among the different calcium solutions was BS (67.3%), with overall bioavailability rates about two times higher than the rates observed in commercially sold calcium supplements and natural calcium. In addition, the in vitro calcium bioavailability rate for ionized calcium in market milk, soy milk, and orange juice was more than twice as high as calcium carbonate. Overall, we expect a high and diverse bioavailability of ionized calcium from natural resources.