Macro-mesoporous scaffolds based on wheat gliadin (WG)/mesoporous magnesium calcium silicate (m-MCS) biocomposites (WMC) were developed for bone tissue regeneration. The increasing amount of m-MCS significantly improved the mesoporosity and water absorption of WMC scaffolds while slightly decreased their compressive strength. With the increase of m-MCS content, the degradability of WMC scaffolds was obviously enhanced, and the decrease of pH value could be slow down after soaking in Tris-HCl solution for different time. Moreover, the apatite mineralization ability of the WMC scaffolds in simulated body fluid (SBF) was obviously improved with the increase of m-MCS content, indicating good bioactivity. The macro-mesoporous WMC scaffolds containing m-MCS significantly stimulated attachment, proliferation and differentiation of MC3T3-E1 cells, indicating cytocompatibility. The WMC scaffold containing 40 w% m-MCS (WMC40) possessed the highest porosity (including macroporosity and mesoporosity), which loaded the highest amount of curcumin (CU) as well as displayed the slow release of CU. The results suggested that the incorporation of m-MCS into WG produced biocomposite scaffolds with macro-mesoporosity, which significantly improved water absorption, degradability, bioactivity, cells responses and load/sustained release of curcumin.