Early-age cracks in fresh concrete occur mainly due to high rate of surface evaporation and restraint offered by the contracting solid phase. Available test methods that simulate severe drying conditions, however, were not originally designed to focus on evaporation and transport characteristics of the liquid-gas phases in a hydrating cementitious microstructure. Therefore, these tests lack accurate measurement of the drying rate and data interpretation based on the principles of transport properties is limited. A vacuum-based test method capable of simulating early-age cracks in 2-D cement paste is developed which continuously monitors the weight loss and changes to the surface characteristics. 2-D crack evolution is documented using time-lapse photography. Effects of sample size, w/c ratio, initial curing and fiber content are studied. In the subsequent analysis, the cement paste phase is considered as a porous medium and moisture transport is described based on surface mass transfer and internal moisture transport characteristics. Results indicate that drying occurs in two stages: constant drying rate period (stage I), followed by a falling drying rate period (stage II). Vapor diffusion in stage I and unsaturated flow within porous medium in stage II determine the overall rate of evaporation. The mass loss results are analyzed using diffusion-based models. Results show that moisture diffusivity in stage I is higher than its value in stage II by more than one order of magnitude. The drying model is used in conjunction with a shrinkage model to predict the development of capillary pressures. Similar approach is implemented in drying restrained ring specimens to predict 1-D crack width development. An analytical approach relates diffusion, shrinkage, creep, tensile and fracture properties to interpret the experimental data. Evaporation potential is introduced based on the boundary layer concept, mass transfer, and a driving force consisting of the concentration gradient. Effect of wind velocity is reflected on Reynolds number which affects the boundary layer on sample surface. This parameter along with Schmidt and Sherwood numbers are used for prediction of mass transfer coefficient. Concentration gradient is shown to be a strong function of temperature and relative humidity and used to predict the evaporation potential. Results of modeling efforts are compared with a variety of test results reported in the literature. Diffusivity data and results of 1-D and 2-D image analyses indicate significant effects of fibers on controlling early-age cracks. Presented models are capable of predicting evaporation rates and moisture flow through hydrating cement-based materials during early-age drying and shrinkage conditions.