Recently, the attention has been drawn to complex systems – biomicroconcretes composed of a bone cement matrix and resorbable granules or microspheres. This paper presents novel bone substitutes composed of α-tricalcium phosphate (α-TCP; cement matrix), calcium sulphate dihydrate granules (GCSD; aggregates in biomicroconcrete) and various polymers (chitosan, sodium alginate, methylcellulose) used for the improvement of material properties. The aim of this work was to study α-TCP-GCSD-polymer interactions and to compare the impact of organic additives on the physicochemical properties of biomicroconcretes. Methods: Scanning electron microscopy (SEM), mercury intrusion porosimetry (MIP), X-ray diffractometry (XRD) as well as universal testing machine (INSTRON), Gilmore apparatus and pH/ conduct-meter were used. Results: The chemical bonding between α-TCP matrix and CSD granules resulted in a compressive strength appropriate for low-load bearing applications (7–12 MPa) and clinically relevant setting times (8–33 min). Biomicroconcretes consisting of sodium alginate possessed the highest mechanical strength (12 ± 2 MPa). It has also been found that the dissolution-precipitation reactions of the α-TCP were retarded with the addition of chitosan and acetic acid. This effect was not observed in the case of methylcellulose and sodium alginate. Chemical stability and bioactivity of materials were demonstrated during in vitro studies in simulated body fluid. Conclusions: Materials containing calcium sulphate-based granules were surgically handy, possessed promising physicochemical properties and are supposed to ensure desired macroporosity as well as gradual resorption in vivo. It has been demonstrated that the presence of CSD granules and polymers influenced the physicochemical properties of composites.