Tissue engineering (TE) is a highly multidisciplinary field that focuses on novel regenerative treatments and seeks to tackle problems relating to tissue growth both in vitro and in vivo. These issues currently involve the replacement and regeneration of defective tissues, as well as drug testing and other related bioapplications. The key approach in TE is to employ artificial structures (scaffolds) to support tissue development; these constructs should be capable of hosting, protecting and releasing bioactives that guide cellular behaviour. A straightforward approach to integrating bioactives into the scaffolds is discussed utilising polyelectrolyte multilayer capsules (PEMCs). Herein, this review illustrates the recent progress in the use of CaCO3 vaterite-templated PEMCs for the fabrication of functional scaffolds for TE applications, including bone TE as one of the main targets of PEMCs. Approaches for PEMC integration into scaffolds is addressed, taking into account the formulation, advantages, and disadvantages of such PEMCs, together with future perspectives of such architectures.