Faced with growing global demand for new potent, bio-based, biocompatible elastomers, the present study reports the solvent-free production of 13 pure and derived poly(glycerol-co-diacid) composite sheets exclusively using itaconic acid, sebacic acid, and 2,5-furandicarboxylic acid (FDCA) with glycerol. Herein, modified melt polycondensation and Co(II)-catalyzed polytransesterification were employed to produce all exploitable prepolymers, enabling the easy and rapid manufacturing of elastomer sheets by extrusion. Most of our samples were loaded with 4 wt% of various additives such as natural polysaccharides, synthetic polymers, and/or 25 wt% sodium chloride as porogen agents. The removal of unreacted monomers and acidic short oligomers was carried out by means of washing with NaHCO3 aqueous solution, and pH monitoring was conducted until efficient sheet surface neutralization. For each sheet, their surface morphologies were observed by Field-emission microscopy, and DSC was used to confirm their amorphous nature and the impact of the introduction of every additive. The chemical constitution of the materials was monitored by FTIR. Then, cytotoxicity tests were performed for six of our most promising candidates. Finally, we achieved the production of two different types of extrusion-made PGS elastomers loaded with 10 wt% PANI particulates and 4 wt% microcrystalline cellulose for adding potential electroconductivity and stability to the material, respectively. In a preliminary experiment, we showed the effectiveness of these materials as performant, time-dependent electric pH sensors when immersed in a persistent HCl atmosphere.