This paper reports an in-depth structural investigation of PdZn nanoparticulates prepared over an entire compositional range. By using a combination of HRTEM, ICP-OES, EDX and XPS alongside PXRD, we are able to show how a liquid-type reduction process can be exploited to target different PdZn bimetallic structures while maintaining reproducibly narrow particle size distributions and average particle diameters of approximately 3 nm. Samples have been further analyzed by quantitative phase analysis of the Rietveld refined diffraction data, providing indications as to how variations in specific surface compositions are obtained when Zn is used as the alloying metal. The influence of nanolattice strain is investigated by geometric analysis of TEM data. Results suggest, in conjunction with previously published catalytic data, how different compositions of this specific bimetallic system may be exploited in catalytic processes to control substrate/product affinity. We thus demonstrate a new and simplified approach to PdZn bimetallics, which may offer novel perspectives for applications in industrial catalysis.