Polysaccharides-based scaffolds for tissue engineering have become a promising field of study, as these biomaterials provide greater biocompatibility and offer lower production costs. In the present study, we describe the development and characterization of scaffolds composed of chitosan (CHT) and cashew gum (CG) in different concentrations, and evaluate their physical and mechanical properties. Molecular docking was used to estimate the intermolecular interactions between CHT and CG. The scaffolds were produced through the solubilization of different ratios of CHT/CG (1:1; 1:0.5 and 1:0.25), and subsequently frozen and lyophilized. The developed scaffolds kept the thermal stability as documented by thermogravimetry (TGA/DTG) and differential scanning calorimetry (DSC) analyses. Fourier transform infrared spectroscopy (FTIR) analysis also showed that functional groups of both CHT and CG were kept in the developed scaffold, while X-ray diffraction (XRD) analysis depicted the typical peaks of semi-crystalline materials of chitosan and wider bands of the amorphous cashew gum. Scanning electron microscopy (SEM) and tomography analyses documented the presence of pores in the three types of scaffolds, with significant sizes that are instrumental for cell proliferation in tissue engineering. Our study demonstrates that, combining CHT and CG, a new biomaterial can be developed for potential applications in tissue engineering, for example, in bone regeneration.