Cationic and anionic polyelectrolytes were investigated for the application as charging agents for the electrophoretic deposition (EPD) of polyetheretherketone (PEEK) and composite coatings, containing huntite or alumina platelets. The use of cationic chitosan (CT) allowed for the fabrication of PEEK coatings by cathodic EPD. Anodic PEEK coatings were prepared using sodium alginate (AL) and poly[1-[4-(3-carboxy-4-hydroxyphenylazo)benzenesulfonamido]-1,2-ethanediyl, sodium salt] (PAZO). The EPD of huntite and PEEK-huntite composites was achieved using AL and PAZO. The EPD of alumina and PEEK-alumina coatings was performed using PAZO. The comparison of the experimental results and molecular structures of AL and PAZO provided an insight into the influence of salicylate ligands of PAZO on adsorption of this polyelectrolyte on inorganic surfaces. The unique physical properties of PAZO, coupled with strong adsorption of this material on organic and inorganic surfaces, pave the way for the fabrication of functional composites by EPD. The deposition mechanism, deposition kinetics and deposit microstructure were investigated. Huntite is advanced flame retardant material with relatively high decomposition temperature, which is of special interest for the incorporation in polymers, such as PEEK, which require thermal processing. It was found that PEEK composites, containing flame retardant huntite additives, can be prepared by EPD. The composite coatings provided corrosion protection of steel. (C) 2015 The Electrochemical Society. All rights reserved.