Hyperspectral remote sensing technology can provide a rapid and nondestructive method for soil nickel (Ni) content detection. In order to select a high-effective method for estimating the soil Ni content using a hyperspectral remote sensing technique, 88 soil samples were collected in Urumqi, northwest China, to obtain Ni contents and related hyperspectral data. At first, 12 spectral transformations were used for the original spectral data. Then, Pearson’s correlation coefficient analysis (PCC) and the CARS method were used for selecting important wavelengths. Finally, partial least squares regression (PLSR), random forest regression (RFR) and support vector machine regression (SVMR) models were used to establish the hyperspectral inversion models of the Ni content in the soil using the important wavelengths. The coefficient of determination (R2), root mean square error (RMSE), mean absolute error (MAE), and residual prediction deviation (RPD) were selected to evaluate the inversion effects of the models. The results indicated that using the PCC and CARS method for the original and transformed wavebands can effectively improve the correlations between the spectral data and Ni content of the soil in the study area. The random forest regression model, based on the first-order differentiation of the reciprocal (RTFD–RFR), was more stable and had the best inversion effects, with the highest predictive ability (R2 = 0.866, RMSE = 1.321, MAE = 0.986, RPD = 2.210) for determining the Ni content in the soil. The RTFD–RFR methods can be used as a means of the inversion of the Ni content in urban soil. The results of the study can provide a technical support for the hyperspectral estimation of the Ni content of urban soil.