A suite of advanced instruments were employed to measure aerosol hygroscopicity, volatility and chemical composition at a suburban site in the Pearl River Delta (PRD) Region and at a marine site in Okinawa, respectively. The results showed that the particle number concentration in PRD is approximately ten times higher than that in Okinawa. Organics contributes about one half of the total NR-PM1 concentration in PRD, while sulfate is the dominant component (about 60%) in Okinawa. Diurnal variation of the chemical species demonstrated that the site in PRD was affected by traffic-related sources and industrial emissions, while the one in Okinawa is mainly affected by regional emissions. The V-TDMA measurements showed that a large fraction (20–45%) of particles in Okinawa volatilized at about 200°C and nearly all particles volatilized at about 300°C, indicating that the particles were almost volatile in Okinawa. In contrast, a fraction (15–21%) of particles in PRD did not evaporate even when heated to about 300°C, implying that these particles might contain black carbon or low-volatile organics. For 40–200 nm particles in Okinawa, the hygroscopicity parameter κ is around 0.5, significantly higher than that of PRD particles (κ ≈ 0.26). Particles tend to have bimodal distribution in PRD and unimodal in Okinawa, indicating that the former is externally mixed while the latter is internally mixed.