Nanoscaled, needle-shaped frequency doublers have been generated via self-assembled surface growth from functionalized quaterphenylene molecules with a designed large hyperpolarizability. The nanofiber frequency doublers exhibit very weak fluorescence centered around 430 nm but emit a strong, resonance-enhanced second-harmonic signal when excited with infrared 80 fs laser pulses. The frequency doublers are employed to correlate second-harmonic response and morphology via two-dimensional true second-harmonic images of individual nanoaggregates obtained with the help of a femtosecond laser scanning microscope.