Boron nitride nanotubes (BNNTs) represent a relatively new class of materials that provides alternative electrical and thermal properties to the carbon analogue. The high chemical and thermal stability and large band gap combined with high electrical resistance make BNNTs desirable in several thin-film applications. In this study, stable BNNT and hexagonal boron nitride (hBN) particle dispersions have been developed using environmentally friendly advanced oxidation processing (AOP) that can be further modified for electrophoretic deposition (EPD) to produce thin films. The characterization of the dispersions has revealed how the hydroxyl radicals produced in AOP react with BNNT/hBN and contaminant boron nanoparticles (BNPs). While the radicals remove the carbon contaminant present on BNNT/hBN and increase dispersion stability, they also oxidize the BNPs and the boron oxide produced, which, conversely, reduces the dispersion stability. The use of high- or low-powered ultrasonication in combination with the AOP affects the rate of the competing reactions, with low-powered sonication and AOP providing the best combination for producing stable dispersions with high concentrations. BNNT/hBN dispersions were functionalized with polyethyleneimine to facilitate EPD, where films of several micrometer thickness were readily deposited onto stainless steel and glass-fiber fabrics. BNNT/hBN films produced on glass fabrics by EPD exhibited a consistent through-thickness macroporosity that was facilitated by platelet and nanotube stacking. The film macroporosity present on the coated fabrics was suitable for use as separator layers in supercapacitors and provided improved device robustness with a minimal impact on electrochemical performance.