For in situ Non-Aqueous Phase Liquid (NAPL) source zone remediation, NZVI must be mobile in porous media and it should have an affinity for the NAPL source zone. There are two methods to promote NAPL targeting, including interfacial targeting where the particles adhere and become immobilized at the NAPL/water interface, and destabilization targeting where a surface coating is desorbed in the presence of NAPL saturation or near-saturation, leaving behind a bare, immobile particle. In this study, we assess the potential of mixtures of an anionic polyelectrolyte, poly(styrene sulfonate) (PSS), and a cationic surfactant, cetyltrimethylammonium bromide (CTAB), as NZVI surface modifiers to enhance NAPL targetability via interfacial targeting or destabilization targeting. Two methods of NZVI surface modification were evaluated; 1) sequential adsorption of CTAB followed by PSS to provide a layered CTAB-seq-PSS structure, and 2) adsorption of a premixed PSS-co-CTAB complex .CTAB-seq-PSS and PSS-co-CTAB modified NZVI dispersions were mixed with excess NAPL (dodecane, TCE, or PCE) in water, or with NAPL-saturated water to evaluate their affinity for the NAPL-water interface (interfacial targeting) and the desorption of PSS and CTAB from NZVI due to the change of solvent quality for the complex (destabilization targeting). Complex desorption and NZVI destabilization in the presence of NAPL was more extensive for the layered CTAB-seq-PSS than for the PSS-co-CTAB complex . Transport of both types of modified NZVI dispersions are through a column of sand partially saturated with NAPL will be discussed to evaluate the potential for in situ NAPL targeting.