We present a newly devised technique, the dynamic layer-by-layer (LbL) deposition method, that is designed to take advantage of the LbL deposition method and fluidic devices. Polyelectrolyte solutions are sequentially injected through the fluidic LbL deposition device to quickly build well-defined multilayer films on a selected region with a linear increase in the material deposited. Multilayer film fabrication by this new method on a specific region was proven to be fast and effective. The effects on film quality of the processing parameters such as concentration of polyelectrolytes, flow rate, and contact time were investigated. A half-tethered self-standing film on a substrate was fabricated to demonstrate the effectiveness and the region-selective deposition capability of the devised dynamic LbL deposition method.