The evaluation of mechanical properties of carbon nanotube (CNT) fibers is inherently difficult. Here, Raman scattering-a generic methodology independent of mechanical measurements-is used to determine the interbundle strength and microscopic failure process for various CNT macroarchitectures. Raman data are used to predict the moduli of CNT films and fibers, and to illustrate the influences of the twisting geometries on the fibers' mechanical performances.