A new method for the patterning of ionic layer-by-layer assembled films with micron-sized features is presented. Self-assembled monolayers (SAMs) were used as templates to direct the deposition of sulfonated polystyrene (SPS) and poly(diallyldimethylammonium chloride) (PDAC) multilayers onto a surface. Both polyelectrolytes were assembled electrostatically from dilute solutions (10 and 20 mM on a repeat unit basis) with varying amounts of sodium chloride. The ionic content was varied from 0 to 4 M NaCl. The optimal conditions for templating were found at moderate salt contents. At high salt contents (greater than or equal to 1 M NaCl) the templating behavior of the chemically patterned SAM surface completely reversed due to electrostatic screening and dehydration of an oligo(ethylene glycol)surface, indicating that ionic strength can be used to dramatically alter polyion deposition behavior on the functionalized surface.