The calcium-induced structuring of pectin solutions has been exploited in many diverse areas of science and technology for many decades, as indeed has controlled calcium release as a methodology for obtaining homogeneous gels in such systems. However, many physical chemistry facets of the release, such as the determination of the rate-limiting step and the explicit investigation of the effects of the ion-binding polymer on the ion release process, have received scant attention. In this work, it is demonstrated that the release of calcium via the controlled dissolution of CaCO3 by GDL can be rate limited either by GDL hydrolysis or by CaCO3 dissolution, dependent on the particle size. The influence of the ion release rate on the gelation of pectin has also been studied, using a methodology to ensure that the resultant mechanical properties of the different systems were all measured at the same pH. Furthermore, for the first time, explicit evidence is provided to support the hypothesis that the presence of the pectin does not significantly influence the dissolution rate of CaCO3.