Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous environmental contaminants known to be hazardous to human health. Pine needles and mosses are useful bio-indicators for assessing PAH pollutions; however, the differences in their PAH uptake mechanisms have not been sufficiently discussed. In this study, the properties of pine needles and mosses as bio-indicators of PAHs were investigated on the basis of differences in their PAH profiles. Five sets each of pine needle and moss samples were collected from circular sampling plots and analyzed for 16 PAHs. A comparison of PAH profiles revealed that the proportion of lower molecular weight PAHs (2 - 3 aromatic rings; LMW PAHs) was significantly higher in pine needles (78.5% ± 4.8%) than in mosses (35.4% ± 6.8%). In contrast, the proportion of higher molecular weight PAHs (5 - 6 aromatic rings; HMW PAHs) was lower in pine needles (4.3% ± 2.9%) than in mosses (25.1% ± 3.3%). Further, the combination of PAH isomer ratios showed that PAH sources between pine needles and mosses were not the same. These differences were explained by their uptake mechanisms and partly by the absorption of PAHs from soil particles by mosses. These findings indicate that pine needles are useful for assessing airborne LMW PAH pollution, whereas mosses can be integrated indicators for assessing complex HMW PAH pollution of the atmospheric and soil environments. On the basis of these properties, the usefulness of these bio-indicators should also be evaluated according to the objective of the assessment and the areas where they are applied.