The tavorite polymorph of LiFeSO4F has recently attracted a lot of interest as a cathode material for lithium ion batteries stimulated by its competitive specific capacity, high potential for the Fe2+/Fe3+ redox couple, and low-temperature synthesis. However, the synthesis routes explored to date have resulted in notably varied electrochemical performance. This inconsistency is difficult to understand given the excellent purity, crystallinity, and similar morphologies achieved via all known methods. In this work, we examine the role of the interfacial chemistry on the electrochemical functionality of LiFeSO4F. We demonstrate that particularly poor electrochemical performance may be obtained for pristine materials synthesized in tetraethylene glycol (TEG), which represents one of the most economically viable production methods. By careful surface characterization, we show that this restricted performance can be largely attributed to residual traces of TEG remaining on the surface of pristine materials, inhibiting the electrochemical reactions. Moreover, we show that optimized cycling performance of LiFeSO4F can be achieved by removing the unwanted residues and applying a conducting polymer coating, which increases the electronic contact area between the electrode components and creates a highly percolating network for efficient electron transport throughout the composite material. This coating is produced using a simple and scalable method designed to intrinsically favor the functionality of the final product.