All-optical processing devices that include patterned optically active polymers. The devices that are constructed according to principles of the invention include at least one optical input port and at least one optical output port, respectively configured to accept optical input signals and provide optical output signals. The devices include optically active material such as organic polymers that interact with illumination at a first wavelength to change at least one optical property in a non-linear manner. The optically active polymer can be placed adjacent one or more waveguides that allow the input illumination to propagate. As the optical property of the optically active material is changed by the incident illumination, the propagating illumination undergoes a modulation or change in phase, thereby providing an optical output signal having a desired relation to the optical input signal, such as the result of a logical or a computational operation.