In recent years the electroreduction of CO₂ to valuable products has emerged as a rational answer to uprising CO₂ emissions and a promising approach to incorporate renewable electricity from intermittent sources into the global energy supply. In particular the reduction of CO₂ to CO has been highlighted in the widely explored industrial conversion of syngas (H₂ and CO) to fuels through subsequent technologies. In this work we report for the first time a strategy to tune the H₂ to CO ratio by facile composition control of the components of a rationally designed binary nanostructure. By adjusting the loading of Au nanoparticles (AuNP) in a 0 to 93 wt.% range immobilized on ultra-thin titanate nanosheets (TiNS), the CO Faradaic efficiency, balanced by an exclusive H₂ formation (HER), could be effectively varied in a 3 to 80% range. Based on gathered XPS characterization, an electronic reconstruction was proposed to dictate the stabilization of formed reaction intermediates and subsequent selectivity to H₂ and CO with these AuNP/TiNS hybrid materials. In addition, with a 73 wt.% Au loading optimally high H₂ and CO production current densities could be achieved at the low cathodic potential region (-0.6 to -0.9 V_RHE). We believe that our novel hybrid nanostructure and its underlying synthesis strategy represent an innovative and promising route to produce syngas with widely tunable H₂ to CO ratios and an industrial platform for a sustainable CO₂ reutilization to products of higher value.