The nonlinear optical response of films of needle-shaped para-hexaphenyl nanoaggregates on mica surfaces is investigated. Two-photon luminescence as well as optical second harmonic generation (SHG) are observed following excitation with femtosecond pulses at 770 nm. Polarization dependent measurements reveal that the nonlinear optical transition dipole moment is oriented with an angle of 75degrees with respect to the needles long axes. The absolute value of the macroscopic second-order susceptibility, averaged over a size distribution of p-6P nanoaggregates, is estimated to be of the order of 6 x 10(-10) esu. (C) 2002 Elsevier Science B.V. All rights reserved.