Water-based high viscosity graphite inks for automated digital deposition of Li-ion battery electrodes have been studied. The flow behaviour and visco-elastic properties of the inks were optimised for a digitally controlled additive manufacturing deposition method and high energy electrodes. A rheology modifier was introduced as an immiscible secondary fluid to control the flow behaviour of these inks. Through optimisation of the formulation, graphite electrodes with high mass loadings were achieved. Depending upon the rheology, both patterned or homogeneously coated electrodes were successfully deposited. The influence of the ink formulation upon the microstructure and electrochemical performance of the prepared anodes is discussed. 3D microstructure was analysed by 2-D electrode cross sectioning and scanning electron microscopy (SEM). It was observed that with an increase of the rheology modifier the alignment of the graphite particles, as well as the distribution of the conductive additive was altered considerably. The dispersion of the conductive additive improved up to 1% additive with greater alignment of the graphite particles, however at 10% additive clumping of the graphite particles was observed. The electrochemical performance of the different electrode microstructures was investigated through electrochemical cycling and impedance spectroscopy. Figure 1 shows the cross-sectional microstructure of the electrodes with 0% and 10% rheology modifier. Figure 1