The spectral structure of harmonics was experimentally controlled by changing the chirp of femtosecond laser pulses, and the dependence of harmonic chirp on atomic species was analysed using harmonics from neon and helium. Experimental results and theoretical analysis based on the Wigner distribution function showed that the spectral structure varied sensitively to laserchirp and the harmonic chirp was determined by the competition between dynamically induced negative chirp and self-phase modulation induced positive chirp. The generation of sharp and bright harmonics was achieved with appropriately chirped laser pulses under given experimental conditions, especially negatively chirped pulses in the case of laser intensity above the saturation intensity for optical-field ionization.