The rapidly increasing deployment of wind and solar energy has resulted in an urgent need for a smarter, more efficient and reliable electronic grid for load balancing. [1,2] Currently, only a small fraction of the total electric production is tied to grid storage, with the vast majority 2 being pumped hydro installations. [3] While the latter technology is mature, cost effective, and efficient, it is geographically limited. [3] Alternate modes of energy storage that can be deployed in a distributed manner include batteries, compressed air, thermochemical energy, and flywheels. [3] Flow batteries are particularly attractive due to their decoupled energy and power, providing design flexibility especially at large scales. [4][5][6] Many flow battery chemistries, however, suffer from limited complex solubility and low nominal voltage, resulting in low energy densities. [7] To overcome this, Duduta et al. developed the semi-solid flow cell (SSFC), [8] in which traditional liquid catholytes and anolytes are replaced by attractive colloidal suspensions composed of Li-ion compounds. They also replaced traditional stationary current collectors with conductive carbon nanoparticle networks within the flowing suspensions. These suspensions, which take advantage of Li-ion battery's high energy density with flow battery's design flexibility, have been investigated both experimentally [8][9][10][11][12] and computationally. [10,13,14] Similar concepts have recently emerged for electrochemical flow capacitors [15] and polysulfide flow batteries. [16] To fully optimize SSFCs, the flowing electrodes must have high active material content coupled with an adequate conductive filler network to overcome the resistive nature of most electrochemically active Li-ion compounds. However, as their solids loading increases, dramatic changes in their rheological properties ensue, which inhibit flow. The key to maximizing active material content while retaining satisfactory flowability and conductivity is to simultaneously tailor the respective interactions between all particles present within these electrode suspensions.[17] 3Here, we report the design and characterization of biphasic SSFC electrode suspensions with high energy density, fast charge transport, and low-dissipation flow. To create these biphasic mixtures [18,19] we specifically tailor the interactions between the active particles, i.e., LiFePO 4 (LFP), to be repulsive, the interactions between the conductive particles, Ketjenblack EC-600JD (KB), to be attractive, and the cross-interactions between LFP-KB to also be repulsive. These two particle populations are suspended and mixed sequentially in propylene carbonate (PC) with 1M of lithium bis(trifluoromethane)sulfonamide (LiTFSI). It is well known that colloidal particles will rapidly aggregate when suspended in polar solvents under high ionic strength conditions due to van der Waals interactions.[20] Hence, we first introduce a non-ionic dispersant, polyvinylpyrrolidone (PVP), with appropriate amount to selectively stabilize ...