A new approach to create layer-by-layer assembled multilayer ultrathin films with welldefined micropatterns in a short process time is introduced. To achieve such micropatterns with high line resolution in organic multilayer films, microfluidic channels were combined with the convective self-assembly process employing both hydrogen bonding and electrostatic intermolecular interactions. The channels were initially filled with polymer solution by capillary pressure and the residual solution was then removed by spinning process. The micropatterns with distinct line boundaries were obtained and the small ridges were also observed at the edges of the patterned lines. Spin self-assembled vertical heterostructural multilayer patterning using (PVP/PAA)5 micropatterns, which were prepared with microfluidic channels, as a template was also investigated.