AbstractInkjet printing of metal nanoparticles allows for design flexibility, rapid processing and enables the 3D printing of functional electronic devices through co-deposition of multiple materials. However, the performance of printed devices, especially their electrical conductivity, is lower than those made by traditional manufacturing methods and is not fully understood. Here, we reveal that anisotropic electrical conductivity of printed metal nanoparticles is caused by organic residuals from their inks. We employ a combination of electrical resistivity tests, morphological analysis and 3D nanoscale chemical analysis of printed devices using silver nanoparticles to show that the polymer stabiliser polyvinylpyrrolidone tends to concentrate between vertically stacked nanoparticle layers as well as at dielectric/conductive interfaces. Understanding the behaviour of organic residues in printed nanoparticles reveals potential new strategies to improve nanomaterial ink formulations for functional printed electronics.