Current (C) and previous year (C + 1) needles and soils (organic horizon, 0-10 cm and 10-20 cm mineral depth) of Masson pine (Pinus massoniana L.) trees were sampled at four forested sites (Huang Pu industrial district, HP; South China Botanical Garden, BG; Mao Feng Mt., MF; and Nan Kun Mt., NK) in Guangzhou along a urban-rural gradient and analyzed for sulfur (S) and heavy metals (Cu, Zn, Ni, Cd, Cr and Pb) concentrations. Needle concentrations of all the elements were significantly higher at industrial HP than at other three sites, except for Cu and Pb which were highest at the traffic site (BG). The C + 1 needles generally had higher Cu, Cd, Pb, Zn, Cr than the C needles while the opposite was for Ni and S. Total and available Cd, Pb, Zn in soils peaked at the urban sites (HP and BG) and decreased at suburban MF and rural NK. Heavy metals were generally higher in the organic soils than in the mineral soils at all sites. Zinc and Pb at all sites, and Cd, S and Cu at the urban sites (HP and BG) in soils or pine needles were above or near their respective natural background levels, implying that threats resulted from these toxic elements occurred on local particularly urban forests, but did not for Cr and Ni due to their presence below their background values. Our results demonstrated that elements concentrations in needles and soils had reflected the variability of pollutants and the environmental quality change along the urban-rural transect, and were efficient as biomonitors to assess the influence of anthropogenic activities along the urbanization course on forest health.