Soil arsenic (AS) contamination has attracted a great deal of attention because of its detrimental effects on environments and humans. AS and inorganic AS compounds have been classified as a class of carcinogens by the World Health Organization. In order to select a high-precision method for predicting the soil AS content using hyperspectral techniques, we collected 90 soil samples from six different land use types to obtain the soil AS content by chemical analysis and hyperspectral data based on an indoor hyperspectral experiment. A partial least squares regression (PLSR), a support vector regression (SVR), and a back propagation neural network (BPNN) were used to establish a relationship between the hyperspectral and the soil AS content to predict the soil AS content. In addition, the feasibility and modeling accuracy of different interval spectral resampling, different spectral pretreatment methods, feature bands, and full-band were compared and discussed to explore the best inversion method for estimating soil AS content by hyperspectral. The results show that 10 nm + second derivative (SD) + BPNN is the optimum method to predict soil AS content estimation; R 2 v is 0.846 and residual predictive deviation (RPD) is 2.536. These results can expand the representativeness and practicability of the model to a certain extent and provide a scientific basis and technical reference for soil pollution monitoring. Sustainability 2020, 12, x FOR PEER REVIEW 3 of 19 polluting enterprises in the suburb, such as chemical plants, funeral homes, medical waste treatment 95 plants, and so on. These polluting enterprises are also direct discharge areas of wastewater, waste 96 gas, and waste slag in Weinan City. In recent years, heavy metal pollution caused by city expansion 97 has drastically affects the soil ecological environment and human health. 98 2.2. Acquisition and Processing of Soil Data 99 The results of previous field investigations indicated that the soil AS content in the mining area 100 is mainly affected by human activities and shows a large difference, and the suburban soil AS 101 content is mainly affected by land use types and shows a small difference. Therefore, from 102 November to December, 2018, 90 soil samples were collected in accordance with the uniform grid 103 method with a higher sampling density in the mining area (50 m) and a lower density in the suburb 104 (200 m). The 50 soil samples were collected from the mining area and the rest form the suburb. There105 were six members in the research group with unified training on the sampling method. First, sample 106 points ware selected on the satellite map, and then the six members were divided into two groups to 107 finish the sampling job in each area. A real-time kinematic (RTK) was used to precisely locate every 108 sampling location. Figure 1 shows the position of the sampling points. The sampling was conducted 109 at a depth of 0-20 cm. Stones, plant residues, and other large debris were removed from each fresh 110 sample, which were then mixed tho...