The rate at which ozone is increasing in the troposphere is uncertain due to the lack of accurate long-term measurements. Old ozone measurements obtained at the Pic du Midi Observatory (3000 m high, southwestern France) were recently rediscovered. Four sets of data available at this station are presented herein: (1) 1874–1881 and (2) 1881–1909 by the Schönbein method and (3) 1982–1984 and (4) 1990–1993 by UV absorption analyzers. The results show an increase in ozone by a factor of 5 since the beginning of the twentieth century, corresponding to an exponential increase of 1.6% per year, although this trend is probably higher (2.4% per year) for the last few decades. A stable 10 ppb ozone mixing ratio is observed during the first 20 years of the series, which is representative of the preindustrial era ozone level. The increase is seen to start around 1895. Other data, obtained at various European high-altitude stations between 1920 and 1980, tie in closely with the Pic du Midi observations. A tentative evaluation of the impact of tropospheric ozone on radiative forcing confirms that ozone is currently the second most significant greenhouse gas, responsible for 22% and 13% of radiative forcing changes since 1800 in the northern and southern hemispheres, respectively. If these rates were to be maintained in the future, ozone would continue to evolve differently in the two hemispheres (maximum level in the northern hemisphere) and could make an even more significant contribution to the radiative forcing of the northern hemisphere.