An integrated and systematic database of sooting tendency with more than 190 kinds of fuels was obtained through a series of experimental investigations. The laser-induced incandescence (LII) method was used to acquire the 2D distribution of soot volume fraction, and an apparatus-independent yield sooting index (YSI) was experimentally obtained. Based on the database, a novel predicting model of YSI values for surrogate fuels was proposed with the application of a machine learning method, named the Bayesian multiple kernel learning (BMKL) model. A high correlation coefficient (0.986) between measured YSIs and predicted values with the BMKL model was obtained, indicating that the BMKL model had a reliable and accurate predictive capacity for YSI values of surrogate fuels. The BMKL model provides an accurate and low-cost approach to assess surrogate performances of diesel, jet fuel, and biodiesel in terms of sooting tendency. Particularly, this model is one of the first attempts to predict the sooting tendencies of surrogate fuels that concurrently contain hydrocarbon and oxygenated components and shows a satisfying matching level. During surrogate formulation, the BMKL model can be used to shrink the surrogate candidate list in terms of sooting tendency and ensure the optimal surrogate has a satisfying matching level of soot behaviors. Due to the high accuracy and resolution of YSI prediction, the BMKL model is also capable of providing distinguishing information of sooting tendency for surrogate design.