Predicting the soluble solid content (SSC) of peaches based on visible/near infrared spectroscopy has attracted widespread attention. Due to the anisotropic structure of peach fruit, spectra collected from different orientations and regions of peach fruit will bring variations in the performance of SSC prediction models. In this study, the effects of spectra collection orientations and regions on online SSC prediction models for peaches were investigated. Full transmittance spectra were collected in two orientations: stem-calyx axis vertical (Orientation1) and stem-calyx axis horizontal (Orientation2). A partial least squares (PLS) method was used to evaluate the spectra collected in the two orientations. Then, each peach fruit was divided into three parts. PLS was used to evaluate the corresponding spectra of combinations of these three parts. Finally, effective wavelengths were selected using the successive projections algorithm (SPA) and competitive adaptive reweighted sampling (CARS). Both orientations were ideal for spectra acquisition. Regions without peach pit were ideal for modeling, and the effective wavelengths selected by the SPA led to better performance. The correlation coefficient and root mean square error of validation of the optimal models were 0.90 and 0.65%, respectively, indicating that the optimal model has potential for online prediction of peach SSC.