Diesel fuel is composed of a complex mixture of hundreds of hydrocarbons that vary globally depending on crude oil sources, refining processes, legislative requirements and other factors. In order to simplify the study of this fuel, researchers create surrogate fuels to mimic the physical and chemical properties of Diesel fuels. This work employed the commercial software Reaction Workbench - Surrogate Blend Optimizer (SBO) to develop a Surrogate Fuel Library containing 18 fuels. Within the fuel library, the cetane number ranges from 35 to 60 (in increments of 5) at threshold soot index (TSI) levels representative of low, baseline and high sooting tendency fuels (TSI = 17, 31 and 48, respectively). The Surrogate Fuel Library provides the component blend ratios and predicted properties for cetane number, threshold soot index, lower heating value, density, kinematic viscosity, molar hydrogen-to-carbon ratio and distillation curve temperatures from T-10 to T-90. A market petroleum Diesel fuel with a cetane number of 50 and a threshold soot index of 31 was selected as the Baseline Diesel Fuel. The combustion, physical and chemical properties of the Baseline Diesel Fuel were precisely matched by the Baseline Surrogate Fuel. To validate the SBO predicted fuel properties, a set of five surrogate fuels, deviating in cetane number and threshold soot index, were blended and examined with ASTM tests. Good agreement was obtained between the SBO predicted and ASTM measured fuel properties. To further validate the Surrogate Fuel Library, key properties that were effected by altering the component blend ratios to control cetane number and TSI were compared to a set of five market Diesel fuels with good results. These properties included density, viscosity, energy density and the T-10 and T-90 distillation temperatures. The Surrogate Fuel Library provided by this work supplies Diesel engine researchers and designers the ability to analytically and experimentally vary fuel cetane number and threshold soot index with fully-representative surrogate fuels. This new capability to independently vary cetane number and threshold soot index provides a means to further enhance the understanding of Diesel combustion and design future combustion systems that improve efficiency and emissions.