Liquid-crystalline (LC) polyfluorenes have been successfully aligned on photoaddressable polymers (PAPs). This is the first example of the alignment of a LC main chain polymer on a photoaligned layer. The degree of molecular alignment in the fluorescent polyfluorene layer on top of an ultra-thin PAP layer is shown to depend strongly on the chemical nature of the PAP. Good alignment with dichroic ratios of more than 10 was only achieved with PAPs containing liquid-crystalline side chains. Patterning with laterally structured alignment was realized in several ways, utilizing reorientation with orthogonally polarized light. Thin PAP layers have further been utilized as hole-conducting alignment layers in polymer light-emitting diodes (LEDs) with polarized emission. In order to facilitate hole transport through the alignment layer, different concentrations of a hole-transporting molecule (HTM) have been mixed into the PAP layer. These hole-conducting alignment layers retained their aligning abilities even at HTM concentrations of 20 wt.-%. LEDs with photometric polarization ratios in emission of up to 14 at a brightness of up to 200 cd/m(2) and an efficiency of 0.3 cd/A could be realized.