In recent decades, thermoelectric (TE) materials have proven to be a complementary source of renewable energy, as they can directly convert waste heat into electrical energy. Energy-efficient, reliable, and scalable synthetic routes for the fabrication of TE materials and their processing into functional devices via low-energy and low-waste routes are necessary for the broader adoption of these materials in various applications. In this work, we report the formulation of hybrid thermoelectric ( h TE) inks based on nanostructured Sb₂Te₃ and Bi₂Te₃, using PMMA as the polymer matrix and hexanedithiol (HDT) as the binder. Percolation studies were conducted to determine the optimal film composition, with an 80% nanoparticle content yielding the highest TE performance. Finite element modelling (FEM) was employed to optimize the device geometry, including the cross-sectional area ratio of p- and n-type legs, to maximize power output. Based on these results, a flexible h TEG was fabricated using the optimized ink composition. The device exhibited an output power of 950 nW and a Power output Density (PoD) of 40.37 nW cm⁻² under a 30 K temperature gradient, significantly outperforming previously reported polymer-based flexible h TEGs incorporating chalcogenides. This study presents a sustainable and effective strategy for developing high-performance hybrid thermoelectric devices through ink formulation, composition optimization, and simulation-guided device design.