Heavy metal (HM) contamination and accumulation is a serious problem around the world due to the toxicity, abundant sources, non-biodegradable properties, and accumulative behaviour of HMs. The degree of soil HM contamination in China, especially in the Yangtze River Delta, is prominent. In this study, 1822 pairs of soil and crop samples at corresponding locations were collected from the southern Yangtze River Delta of China, and the contents of Ni, Cr, Zn, Cd, As, Cu, Hg, and Pb were measured. The single pollution index in soil (SPI) and Nemerow composite pollution index (NCPI) were used to assess the degree of HM pollution in soil, and the crop pollution index (CPI) was used to explore the degree of HM accumulation in crops. The bioaccumulation factor (BAF) was used to investigate the translocation of heavy metals in the soil-crop system. The health risks caused by HMs were calculated based on the model released by the U.S. Environmental Protection Agency. The SPIs of all elements were at the unpolluted level. The mean NCPI was at the alert level. The mean CPIs were in the following decreasing order: Ni (1.007) > Cr (0.483) > Zn (0.335) > Cd (0.314) > As (0.232) > Cu (0.187) > Hg (0.118) > Pb (0.105). Only the mean content of Ni in the crops exceeded the national standard value. The standard exceeding rates were used to represent the percentage of samples whose heavy metal content is higher than the corresponding national standard values. The standard exceeding rates of Cu, Hg, and Cd in soil were significantly higher than corresponding values in crops. Meanwhile, the standard exceeding rates of Ni, As, and Cr in crops were significantly higher than corresponding values in soil. The chronic daily intake (CDI) of children (13.8 × 10−3) was the largest among three age groups, followed by adults (6.998 × 10−4) and seniors (5.488 × 10−4). The bioaccumulation factors (BAFs) of all crops followed the order Cd (0.249) > Zn (0.133) > As (0.076) > Cu (0.064) > Ni (0.018) > Hg (0.011) > Cr (0.010) > Pb (0.001). Therefore, Cd was most easily absorbed by crops, and different crops had different capacities to absorb HMs. The hazard quotient (HQ) represents the potential non-carcinogenic risk for an individual HM and it is an estimation of daily exposure to the human population that is not likely to represent an appreciable risk of deleterious effects during a lifetime. All the HQs of the HMs for the different age groups were significantly less than the alert value of 1.0 and were at a safe level. This indicated that citizens in the study area face low potential non-carcinogenic risk caused by HMs. The total carcinogens risks (TCRs) for children, adults, and seniors were 5.24 × 10−5, 2.65 × 10−5, and 2.08 × 10−5, respectively, all of which were less than the guideline value but at the alert level. Ingestion was the main pathway of carcinogen risk to human health.