The concurrent release of calcium phosphate and biomacromolecules may improve wound healing responses at the interface with ceramic materials of orthopaedic and dental implants. Hydrogel coatings consisting of a mixture of alginate and chitosan were doped and applied onto solid carriers with the aim of investigating their use as local delivery vehicles. Coatings containing both the model macromolecule FITC-dextran 70 kDa (FD 70) and dispersed calcium phosphate carbonate (CPC) nanoparticles were coated onto a solid, nonporous model substrate to study the concurrent release of FD 70 and calcium and phosphate ions from within the hydrogel. Hydrogel coatings containing only FD 70 were cast onto porous calcium phosphate coatings, similar to hydroxyapatite, to study the release of FD 70 from, and calcium and phosphate ions through, the hydrogel coating. Transmission electron microscopy showed good dispersion of the CPC nanoparticles, and scanning electron microscopy and atomic force microscopy showed that increased CPC loading resulted in an increase in surface roughness but to extents well below those affecting cell responses. The release of FD 70 from CPC-loaded coatings was similar to release from the hydrogel alone, although higher CPC loadings resulted in small changes. The release of FD 70 was better described by double or triple phase zero order release kinetics; this complex time dependence indicates that in addition to outdiffusion, other, time-dependent factors apply, such as swelling of the gel, as expected from the known effects of calcium ions on alginate. Calcium and phosphate ions were also released, with similar release kinetics, through the hydrogel layer from the underlying CaP layer. In either case, release decreased to negligible levels after 3 days, suggesting that the systems of this study are suitable for short-term concurrent release of water-soluble biomacromolecules and calcium and phosphate ions.