The soil particle-size fractions (PSFs) are one of the most important attributes to influence soil physical (e.g., soil hydraulic properties) and chemical (e.g., cation exchange) processes. There is an increasing need, therefore, for high-resolution digital prediction of PSFs to improve our ability to manage agricultural land. Consequently, use of ancillary data to make cheaper high-resolution predictions of soil properties is becoming popular. This approach is known as “digital soil mapping.” However, most commonly employed techniques (e.g., multiple linear regression or MLR) do not consider the special requirements of a regionalized composition, namely PSF; (1) should be nonnegative (2) should sum to a constant at each location, and (3) estimation should be constrained to produce an unbiased estimation, to avoid false interpretation. Previous studies have shown that the use of the additive log-ratio transformation (ALR) is an appropriate technique to meet the requirements of a composition. In this study, we investigated the use of ancillary data (i.e., electromagnetic (EM), gamma-ray spectrometry, Landsat TM, and a digital elevation model to predict soil PSF using MLR and generalized additive models (GAM) in a standard form and with an ALR transformation applied to the optimal method (GAM-ALR). The results show that the use of ancillary data improved prediction precision by around 30% for clay, 30% for sand, and 7% for silt for all techniques (MLR, GAM, and GAM-ALR) when compared to ordinary kriging. However, the ALR technique had the advantage of adhering to the special requirements of a composition, with all predicted values nonnegative and PSFs summing to unity at each prediction point and giving more accurate textural prediction.