The present work aims to develop new biocomposites based on gelatin (Gel) and poly(vinyl alcohol) (PVA) reinforced with graphene oxide (GO). On the one hand, the model is designed with consideration of the high performance of the aforementioned biopolymers as biomaterials; on the other hand, the original component of the system, GO, is expected to improve structural stability and boost mechanical strength. Porous Gel–PVA/GO materials with GO content ranging from 0.5 to 3 wt% are obtained by freeze-drying. Structural analysis by Fourier transform infrared spectrometry (FT-IR), X-ray diffraction (XRD) and transmission electron microscopy (TEM) revealed the ability of well-dispersed GO nanosheets to form interactions with the polymers, leading to a unique molecular structuration. 3D analysis by X-ray microtomography (microCT) and scanning electron microscopy (SEM) suggests that GO has an influence on pore adjustment. According to mechanical tests, GO undoubtedly exhibits a beneficial effect on the polymer resistance against compressive stress, improving their compressive strengths by 97–100% with the addition of 0.5–3 wt% GO. Moreover, biological assessment using the MC3T3-E1 preosteoblast murine cell line indicated the fabrication of a cytocompatible composite formula, with potential for further in vivo testing and tissue engineering applications.