Organic dipolar molecules have attracted much interest over the past decades because of their very large nonlinear optical (NLO) response, holding promise for applications in photonics. Yet, a long standing issue is that to achieve a macroscopic NLO response, the asymmetry intrinsic to dipolar molecules needs to be extended from the molecular scale, over the supramolecular mesoscale, all the way to the macroscopic scale – yet dipole-dipole interactions tend to favor a pairwise anti-parallel orientation in a bulk material, thus cancelling the molecular NLO responses. In this project, three groups will join forces to combine two novel experimental concepts with multiscale modelling to tackle this alignment problem at the nano-, meso- and macro-scales simultaneously: As recently demonstrated for the first time at UAntwerp, dipolar NLO molecules spontaneously adopt an ideal head-to-tail alignment when confined as one-dimensional arrays inside carbon nanotubes. This concept will be elaborated to form highly dipolar NLO nanohybrids and combined with the technique of electrospinning, core expertise of the UGent group, to align the nanohybrids also at the mesoscale in nanofibers. Then, these nanofibers will be aligned in turn on the macroscopic scale to form NLO films. The whole process will be modelled at the KULeuven group in a multiscale approach, from atomistic simulations of the molecular alignment to large scale coarse grained calculations of the alignment of the nanohybrids.