Highly porous three-dimensional polylactide (PLA) scaffolds were obtained from PLA incorporated with different amounts of chitosan-modified montmorillonite (CS-MMT), through solvent casting and particulate leaching method. The processed scaffolds were tested in vitro for their possible application in bone tissue engineering. Scaffolds were characterized by focused ion beam scanning electron microscopy (FIB SEM), fourier transform infra-red (FTIR), X-ray diffraction (XRD), thermogravimetric analysis (TGA), and differential scanning calorimetry (DSC) to study their structure, intermolecular interactions, and thermal properties. Bioresorbability tests in simulated body fluid (pH 7.4) were conducted to assess the response of the scaffolds in a simulated physiological condition. The FIB SEM images of the scaffolds showed a porous architecture with gradual change in morphology with increasing CS-MMT concentration. FTIR analysis revealed the presence of both PLA and CS-MMT particles on the surface of the scaffolds. XRD showed that the crystalline unit cell type was the same for all the scaffolds, and crystallinity decreased with an increase in CS-MMT concentration. Thermal analysis of the scaffolds showed that the incorporation of the CS-MMT particles enhanced the thermal stability of the scaffolds. The scaffolds were found to be bioresorbable, with rapid bioresorbability on the scaffolds with a high CS-MMT concentration. Human fetal osteoblasts (hFOBs) were seeded on the scaffolds to evaluate the extent of cell adhesion and the effect of the CS-MMT on the bioactivity of the PCL scaffolds. Further, osteogenic differentiation of hFOBs on the PLA/CS-MMT scaffolds was studied by analysing the alkaline phosphatase activity on the cell-seeded substrates.